Engineering GaN-based systems for photocatalysis: strategies and applications

Kun Wang, Yunchao Lei, Zefei Wu, Mengyang Zhang, Ting Zhi* and Longlu Wang*
College of Electronic and Optical Engineering, Institute of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications (NJUPT), Nanjing 210023, Jiangsu, P. R. China. E-mail: 1223025002@njupt.edu.cn; 1223024938@njupt.edu.cn; B22021922@njupt.edu.cn; b22020220@njupt.edu.cn; zhit@njupt.edu.cn; wanglonglu@hnu.edu.cn

First published on 15th August 2025

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1. Introduction

Photocatalysis serves as a fundamental pillar of modern science and industrial systems, playing a critical role in fields such as energy conversion, environmental remediation, and chemical synthesis.^1–4 By reducing activation energies and enhancing reaction rates and selectivity,^5–7 catalytic processes significantly improve energy utilization efficiency, driving advancements in green chemistry and sustainable technologies.⁸ The development of efficient and stable photocatalytic materials is crucial for realizing clean energy production and environmental pollution control.^9,10 Therefore, the exploration of high-performance semiconductor photocatalytic materials has become a key focus of current catalysis research.

Gallium nitride based photocatalytic materials have evolved from UV-active semiconductors to advanced systems with improved visible-light response, achieved through doping, nanostructuring, and heterojunction engineering.¹¹ These advances have expanded their applications from water splitting to CO₂ reduction, N₂ fixation and pollutant degradation, highlighting GaN's potential in solar-driven catalytic technologies.^12–14 Gallium nitride (GaN), a typical III–V semiconductor with a hexagonal wurtzite structure, possesses a direct bandgap of approximately 3.4 eV that spans the redox potentials of proton reduction and water oxidation. This alignment allows GaN to effectively harness ultraviolet light while exhibiting exceptional chemical and thermal robustness.¹⁵ These properties allow GaN to maintain excellent performance even under extreme conditions, demonstrating its inherent advantages as a photocatalytic material. Compared to conventional semiconductor materials such as TiO₂ (bandgap ∼3.2 eV),¹⁶ SiC (indirect bandgap),¹⁷ and g-C₃N₄ (narrow bandgap and limited stability),¹⁸ GaN exhibits higher chemical inertness and corrosion resistance, and its polarization properties induce spontaneous internal electric fields that further promote efficient separation of photogenerated electron–hole pairs.¹⁹ These superior physical and chemical properties endow GaN with unique and outstanding application potential in the field of photocatalysis.

Benefiting from its excellent electronic structure and high stability, GaN materials have demonstrated broad application prospects in key photocatalytic reactions such as water splitting for hydrogen production, CO₂ photoreduction to fuels, and organic pollutant degradation. In recent years, with advances in nanostructure engineering, doping modification, heterostructure construction, and surface defect engineering, GaN-based catalytic systems have achieved significant improvements in light absorption range, catalytic activity, and stability. In photocatalytic applications, GaN-based materials have particularly exhibited outstanding performance in areas such as water splitting for hydrogen production, CO₂ reduction, pollutant degradation, and organic transformation. Further exploration and optimization of the photocatalytic performance of GaN materials are of great scientific significance and practical value for advancing efficient energy conversion and environmental remediation technologies.

2. Strategies for modulating the photocatalytic performance of GaN

A variety of optimization strategies have been proposed to enhance the photocatalytic performance of GaN. Nanowire and porous structure designs can significantly increase the specific surface area of GaN, expose more catalytic active sites, shorten charge transport pathways, reduce electron–hole recombination, and thus enhance photocatalytic efficiency.^20–24 Element doping regulates the band structure, optimizes the conduction and valence band positions, broadens the light absorption range, and enhances visible-light responsiveness.²⁵ Constructing heterostructures, such as combining GaN with ZnO or InGaN, can create built-in electric fields at the interface, effectively facilitating the spatial separation of photogenerated electrons and holes and improving charge utilization.^26–28 Surface engineering, particularly through the introduction of defects such as nitrogen or gallium vacancies, can regulate the surface electronic structure, activate catalytic sites, and steer specific reaction pathways, thereby enhancing reaction selectivity and rate.^29–31 The integrated application of these strategies provides a solid theoretical foundation and technical support for developing efficient and stable GaN-based photocatalytic systems.

2.1. Structure design

The nanostructure design of GaN including nanowires/nanosheets and porous structures, plays a crucial role in optimizing active site exposure and enhancing charge carrier transport efficiency.²⁰ The nanowire/nanosheet structure, with its high aspect ratio, offers an increased specific surface area, thereby exposing more catalytic active sites.³² Additionally, its one-dimensional electron transport pathway enhances charge carrier mobility and suppresses electron–hole recombination, leading to improved photocatalytic performance. Furthermore, the porous GaN structure, characterized by nanoscale pores, significantly enhances active site exposure and facilitates reactant diffusion, thereby improving catalytic efficiency.³³ Moreover, the porous structure can generate an intrinsic electric field gradient that promotes electron–hole separation while providing multidirectional charge transport pathways, contributing to an enhanced photocurrent response.

2.2. Element doping

Element doping is a key strategy for tuning the band structure and optical absorption range of semiconductors, effectively enhancing their photocatalytic performance.^25,40 By introducing specific impurity elements, doping can alter the conduction and valence band positions, thereby optimizing the bandgap structure and extending the optical absorption range.⁴¹ A well-designed doping strategy enables precise control over the band structure, broadens the spectral response, and enhances photogenerated charge carrier utilization, thereby improving material performance in photocatalysis.

Surface band bending plays a crucial role in regulating the spatial separation of photogenerated electrons and holes. Doping techniques can effectively modulate the positions of the valence and conduction bands in semiconductors.^44,45 Although surface band bending significantly influences redox reactions, achieving optimal photocatalytic performance still requires rational design and tuning of the semiconductor band structure.⁴⁶ In photocatalytic water splitting, as illustrated in Fig. 3(a), n-type semiconductors typically exhibit upward band bending, driving photogenerated electrons into the bulk and thereby reducing the apparent quantum efficiency. In contrast, p-type semiconductors display downward band bending, favoring the accumulation of electrons at the surface reaction sites and facilitating water splitting. As shown in Fig. 3(b), the construction of multilayer Mg-doped p-type GaN/InGaN nanowire heterostructures enables the formation of a dual-band system, allowing for synergistic utilization of UV and visible photons to enhance solar energy harvesting. The inset of Fig. 3(b) shows that GaN and InGaN have bandgaps of 3.4 eV and 2.61 eV, respectively, corresponding to two interband photoluminescence (PL) peaks at 364 nm and 475 nm in Fig. 3(c). Furthermore, as shown in Fig. 3(d), increasing the Mg doping concentration leads to a gradual decrease in the energy difference between the Fermi level and valence band maximum (E_FS − E_VS) of InGaN. The broad tunability of the surface Fermi level in InGaN nanowires (approximately 1.7 eV) offers a significant opportunity to achieve nearly flat band alignment with water redox potentials. This band structure facilitates the rapid diffusion of photogenerated electrons and holes to the surface, enabling efficient and balanced surface redox reactions.

When the surface of n-type GaN comes into contact with water, its upward band bending becomes more pronounced, as shown in Fig. 3(e) and (f), which suppresses the water reduction reaction. In contrast, when the surface of p-type GaN reaches equilibrium with water, the degree of downward band bending may increase, as shown in Fig. 3(g) and (h), thereby limiting the water oxidation reaction. In practice, the surface of p-type doped GaN nanowires often exhibits weak n-type or nearly intrinsic characteristics, with the Fermi level located slightly above the electrochemical potential of water. Therefore, upon contact with water and achieving energy level equilibrium, the originally downward band bending in such GaN nanowires may be reduced. By tuning the surface Fermi level of the nanowires, more balanced and efficient redox reactions may be achieved. Mi et al. significantly enhanced the photocatalytic performance of GaN nanowires by introducing p-type Mg doping to regulate the near-surface band bending.⁴² In their study, the band structure near the nanowire surface was estimated by measuring the energy difference between the Fermi level (E_F) and the valence band maximum (E_V).⁴³ As shown in Fig. 3(i), Regions I and II correspond to n-type and p-type surfaces, respectively. The reduction in E_F − E_V in the near-surface region is directly associated with the decreased downward band bending resulting from increased Mg doping concentration. Furthermore, the study indicates that variations in surface band bending exhibit minimal dependence on the morphology of GaN nanowires and can be considered negligible.

In summary, effective modulation of the surface Fermi level to reduce downward band bending can significantly enhance the photocatalytic performance of GaN nanowires.

2.3. Heterostructure construction

Constructing GaN-based heterostructures is an effective strategy to enhance the separation efficiency of photogenerated charge carriers. Although GaN possesses a wide bandgap and excellent stability, it suffers from a high recombination rate of photogenerated electrons and holes, which limits its photoelectric conversion efficiency. By integrating GaN with semiconductors that possess complementary band edge positions (e.g., ZnO, InS, PtSe₂, or TiO₂), significant conduction and valence band offsets can be formed, generating strong built-in electric fields or band alignments that drive photogenerated electrons and holes to separate material interfaces, thereby greatly reducing recombination and improving spatial charge separation.^26,47,48 Moreover, polarization effects in GaN-based heterojunctions, such as piezoelectric and spontaneous polarization, can further enhance the interfacial built-in electric field, thereby promoting charge separation.⁴⁹ Therefore, careful engineering of GaN heterostructures can effectively improve their photocatalytic performance.

Fig. 4(a) and (b) show schematic representations of the atomic structures of PtSe₂ and GaN, respectively.⁵⁰ To better understand their electronic properties, the projected density of states (PDOS) of PtSe₂ and GaN were analyzed. As shown in Fig. 4(c), monolayer PtSe₂ exhibits an indirect bandgap, with the valence band maximum (VBM) located at the Γ point in the first Brillouin zone, and the conduction band minimum (CBM) positioned between the Γ and K points, resulting in a bandgap of 2.13 eV. Fig. 4(d) shows the band structure of monolayer GaN, where both the VBM and CBM are located at the Γ point, indicating a direct bandgap of 4.39 eV. PDOS analysis indicates that in monolayer PtSe₂, the VBM is primarily dominated by Se-p orbitals, while the CBM is mainly contributed by Se-p and Pt-d orbitals. In contrast, for monolayer GaN, the VBM is primarily derived from N-p states, while the CBM is composed of N-s and Ga-s states. Hui et al. designed a van der Waals (vdW) heterostructure composed of monolayer GaN and monolayer InS to achieve efficient spatial separation of photogenerated charge carriers.⁵¹ This heterostructure enables oxidation and reduction reactions to occur at separate material interfaces, suppressing electron–hole recombination and thereby enhancing photocatalytic efficiency.^52,53 Multiple stacking configurations of the GaN/InS vdW heterostructure can be formed, including the representative H1 structure, as illustrated in Fig. 4(e)–(j). Analysis of the projected band structure (Fig. 4(k)) reveals a bandgap of 1.91 eV, with the VBM primarily derived from GaN and the CBM mainly contributed by InS. Further PDOS analysis (Fig. 4(l)) indicates that the VBM consists mainly of N-p and Ga-d orbitals, while the CBM is contributed by In-s and S-p orbitals. These results confirm that the heterostructure is an indirect bandgap semiconductor, which favors prolonged carrier lifetimes and thus enhances photocatalytic performance. In the heterostructure, a significant conduction band offset (CBO) and a relatively small valence band offset (VBO) together create a favorable band alignment for charge separation. Under solar illumination, photogenerated electrons in the GaN layer are driven by the CBO to migrate to the InS layer, while holes in the InS layer migrate toward the GaN layer under the influence of the VBO. As shown in Fig. 4(m), the electrostatic potential of the InS layer is lower than that of the GaN layer along the Z direction, resulting in a potential barrier of approximately 1.10 eV. This built-in electrostatic potential gradient efficiently promotes electron transfer to the InS monolayer and hole migration to the GaN monolayer, significantly suppressing carrier recombination and ultimately enhancing the photocatalytic performance of the heterostructure.

2.4. Surface engineering

Surface defect engineering of GaN is an effective material modification strategy that allows precise regulation of reaction pathways in photocatalytic processes.^29–32,54 Surface defects in GaN crystals, including nitrogen or gallium vacancies, dangling bonds, and interstitial atoms, can substantially increase the density of catalytic active sites, tune surface electronic states and band-edge positions, and reduce activation energy, thus promoting targeted redox processes.^55–57 Furthermore, by controlling the type and concentration of defects, new intermediate energy levels or trap states can be introduced on the GaN surface, optimizing the capture and release dynamics of charge carriers, extending their lifetimes, and suppressing electron–hole recombination.^58,59 Rational design of surface defect structures in GaN can effectively direct photogenerated electrons or holes to selectively participate in target reactions (e.g., proton reduction for hydrogen evolution) while suppressing undesired side reactions, thereby improving both the overall photocatalytic efficiency and reaction selectivity. Therefore, GaN surface defect engineering offers a critical approach for modulating reaction pathways to enhance photocatalytic performance.

Surface defects are widely recognized as dominant recombination centers for photogenerated charge carriers, posing a substantial barrier to efficient photocatalysis. To mitigate this challenge, Liu et al. implemented thermal annealing, which substantially suppressed surface defect density in GaN:ZnO particles.⁶⁰ Fig. 5(a) displays the ultraviolet-visible (UV-Vis) absorption spectra of ZnO and GaN:ZnO solid solutions. A pronounced red shift in the absorption edge is observed for GaN:ZnO relative to ZnO, signifying enhanced optical absorption. This shift is attributed to an upward displacement of the valence band induced by the higher ZnO content, effectively narrowing the bandgap. To gain deeper insights into the semiconductor properties and band alignment, Mott–Schottky analysis was performed in an electrolyte with pH 4.0, revealing a bandgap of ∼2.3 eV and enabling extrapolation of the conduction and valence band positions (Fig. 5(b)). As depicted in Fig. 5(c), the band alignment of GaN:ZnO—with both the CBM and VBM spanning the redox window of water—fulfills the thermodynamic prerequisites for overall photocatalytic water splitting.

Due to their relatively narrow bandgaps, oxynitrides are widely regarded as promising photocatalytic materials. However, nitrogen vacancies, which are readily formed during synthesis, serve as recombination centers for photogenerated electrons and holes, significantly reducing photocatalytic activity. To address this issue, Kaveh et al. employed high-pressure torsion (HPT) treatment on GaN:ZnO oxynitrides, aiming to convert detrimental nitrogen vacancies into nitrogen-based vacancy complexes.⁶¹ Fig. 5(d) illustrates a schematic of the HPT processing mechanism. After treatment, the GaN:ZnO sample color changed from yellow to magenta (Fig. 5(e)), accompanied by a shift in the absorption edge from the blue to the green region. As shown in Fig. 5(f), the photoluminescence (PL) peak intensity of the HPT-processed GaN:ZnO sample is significantly reduced, indicating that the reduced concentration of nitrogen vacancies effectively suppresses carrier recombination. Compared to isolated nitrogen vacancies, the nitrogen-based vacancy complex greatly reduced electron–hole recombination, thereby improving the effective utilization of charge carriers.^62,63 The electron paramagnetic resonance (EPR) spectrum in Fig. 5(g) further confirms the formation of nitrogen-based vacancy complexes. The evolution of the electronic structure is further clarified by the UV–Vis absorption spectra (Fig. 5(h)) and the Kubelka–Munk plot (Fig. 5(i)). Following HPT treatment, the absorption edge of the material redshifts from the blue to the green region, with the bandgap narrowing from 2.7 eV to 2.4 eV, indicating that the formation of nitrogen-based vacancy complexes effectively tunes the band structure and enhances visible light absorption.^64–66

In summary, nitrogen-based vacancy complexes introduced via mechanical strain transform conventionally detrimental nitrogen vacancies into functional defects that facilitate charge separation and redox reactions, thereby significantly enhancing the photocatalytic performance of GaN:ZnO oxynitrides.

3. Applications of GaN in photocatalysis

GaN, with its wide bandgap, remarkable thermal and chemical stability, and superior optoelectronic characteristics, has substantial promise across a broad spectrum of photocatalytic applications.^22,39,67,68 In the context of photocatalytic water splitting, GaN's appropriate band-edge positions and spontaneous polarization enhance the separation of photogenerated carriers, thereby driving efficient hydrogen evolution. For photocatalytic CO₂ reduction, surface band engineering and cocatalyst integration allow GaN to selectively convert CO₂ into high-energy-density fuels such as CH₄. GaN also exhibits considerable capability in photocatalytic nitrogen fixation, facilitating the direct conversion of molecular N₂ into NH₃ under mild conditions. In environmental remediation, GaN's strongly oxidative photogenerated holes enable the effective degradation of persistent organic pollutants, ensuring efficient purification of contaminated water or air. Moreover, GaN is capable of activating inert chemical bonds, thereby enabling green and sustainable pathways for selective organic syntheses. The rational design of nanostructures, elemental doping, and heterojunction formation has continuously enhanced GaN's photocatalytic efficiency, reinforcing its pivotal role in clean energy generation and environmental restoration.

3.1. Photocatalytic water splitting for hydrogen production

Overall water splitting (OWS), achieved without external bias or sacrificial agents, directly decomposes water into hydrogen and oxygen in a 2:1 molar ratio, and is considered a long-term, clean, and sustainable approach to solar fuel production.^69,70 In contrast to photoelectrochemical water splitting systems that require strong acidic or alkaline electrolytes and applied voltage, photocatalytic OWS can utilize freshwater or even seawater as the reaction medium without external energy input, thereby greatly reducing system complexity, operating costs, and corrosion-related stability issues.^20,71–73 However, photocatalytic OWS still faces critical challenges, including a narrow visible-light response range, severe recombination of photogenerated electrons and holes, high overpotentials for catalytic reactions, and surface recombination of the evolved gases.^74,75 These limitations collectively constrain the overall system efficiency, resulting in current solar-to-hydrogen (STH) conversion efficiencies typically below 3%.⁷⁶ Although some UV-responsive photocatalysts (e.g., Al-doped SrTiO₃) have demonstrated high quantum efficiencies, the contribution of UV light is minimal in practical applications as it accounts for only ∼3% of the solar spectrum. In contrast, effective utilization of visible light (∼40%) and infrared light (∼50%), which comprise the majority of solar energy, remains the key to improving STH efficiency.^77,78 Recently, InGaN/GaN nanowire photocatalysts grown on silicon substrates have emerged as ideal candidates for efficient OWS, owing to their broad visible-light response (400–700 nm) and favorable band structure. These materials exhibit both excellent light-harvesting capabilities and efficient charge carrier separation, offering a new technological pathway to overcome the current limitations of OWS.^79–82 As shown in Table 1, the STH of various GaN-based systems.

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InGaN/GaN nanowire arrays were successfully synthesized on silicon substrates via MBE. Field emission scanning electron microscopy (FESEM) images (Fig. 6(a)) reveal that the nanowires are uniformly structured and well-aligned on the silicon substrate.^86–88 Rh/Cr₂O₃ core–shell structures and Co₃O₄ nanoparticles were photo-deposited onto the surface of the InGaN/GaN nanowires (Fig. 6(b)) to serve as cocatalysts for hydrogen and oxygen evolution, respectively. The Rh/Cr₂O₃ core–shell structure functions as a reduction cocatalyst to promote proton reduction for hydrogen generation, while Co₃O₄ acts as an oxidation cocatalyst to accelerate hole-mediated oxygen evolution from water.^89,90 When both cocatalysts are present on the photocatalyst surface, they function as electron and hole traps, respectively, enabling efficient spatial separation of charge carriers and significantly suppressing electron–hole recombination, thereby enhancing overall photocatalytic performance.^78,91 The synergistic effect between the reduction and oxidation cocatalysts not only enhances the hydrogen evolution rate but also ensures the continuity and stability of the overall water splitting reaction.

Mi et al. reported a pronounced temperature-dependent hydrogen–oxygen recombination effect in InGaN/GaN nanowire photocatalysts loaded with Rh/Cr₂O₃/Co₃O₄ cocatalysts.⁸³ They proposed a synergistic mechanism in which elevated temperatures simultaneously promote forward hydrogen and oxygen evolution reactions while inhibiting the reverse hydrogen-oxygen recombination process in photocatalytic OWS (Fig. 6(c)). This observation underscores the critical role of reaction temperature in governing the gas evolution dynamics during OWS. Based on their experimental findings, the researchers proposed an efficient reaction pathway and further demonstrated that the system achieved a solar-to-hydrogen (STH) conversion efficiency of approximately 9.2% at an optimal temperature of ∼70 °C. The enhanced performance is primarily attributed to improved forward reaction kinetics and effective suppression of recombination between hydrogen and oxygen, leading to significantly higher hydrogen production efficiency and improved reaction selectivity.^92,93

Generally, elevating the reaction temperature enhances mass transport and promotes both the formation and cleavage of chemical bonds during catalytic reactions, thus contributing to improved reaction rates. In pure water OWS within the 30 °C to 80 °C range, the STH efficiency of Rh/Cr₂O₃/Co₃O₄-loaded InGaN/GaN nanowires displays a strong dependence on the system's operating temperature, rising notably with increasing temperature (Fig. 6(d)). However, raising the temperature beyond 80 °C does not yield a further increase in STH efficiency. Thus, temperature emerges as a critical determinant of the STH efficiency in the photocatalytic OWS system employing Rh/Cr₂O₃/Co₃O₄-decorated InGaN/GaN nanowires presented herein. Under concentrated simulated solar irradiation (Fig. 6(e)), a 74-hour test yielded an STH efficiency of 9.2% with pure water. A hydrogen–oxygen recombination experiment was devised to elucidate the temperature-dependent behavior of the recombination process (Fig. 6(f)). At different temperatures under identical illumination conditions, stoichiometric amounts of hydrogen and oxygen were initially generated. Upon discontinuation of light exposure, the hydrogen and oxygen concentrations decreased progressively over time with an approximate 2:1 stoichiometric ratio, directly confirming hydrogen–oxygen recombination.⁹⁴ Notably, the equilibrium concentrations of hydrogen and oxygen exhibited a pronounced temperature dependence. The hydrogen–oxygen equilibrium concentrations increased with rising temperature, reaching a maximum at approximately 70 °C.

To gain deeper insight into the atomic-scale mechanisms underlying temperature-dependent hydrogen–oxygen recombination, density functional theory (DFT) calculations were conducted to elucidate the reaction pathways occurring on the cocatalyst. As illustrated in Fig. 6(g), the hydrogen–oxygen recombination barrier on Rh is substantially lower compared to Cr₂O₃/Co₃O₄, identifying Rh as the dominant recombination center. Furthermore, the recombination of hydrogen and oxygen on Rh is predominantly exothermic, suggesting that moderate temperature elevation within a defined range can effectively inhibit this recombination process. However, upon further elevation to 80 °C, hydrogen–oxygen recombination predominates once again, reinforcing the conclusion that 70 °C is the optimal temperature for suppressing recombination on InGaN/GaN NWs.^95–97

In conclusion, the present study establishes 70 °C as the optimal reaction temperature for the GaN-based photocatalytic system. For practical industrial-scale hydrogen production applications, this temperature demonstrates promising potential as the operational condition for GaN-based NW photocatalytic systems.

3.2. Photocatalytic CO₂ reduction

The chemical conversion of carbon dioxide (CO₂) presents a promising strategy to address various global challenges, including energy storage, energy scarcity, and environmental issues arising from escalating greenhouse gas emissions.^98–101 Unlike photoelectrochemical CO₂ reduction techniques that require an external voltage supply, photocatalytic reduction typically depends solely upon CO₂, sunlight, and water, thereby mimicking the natural photosynthesis processes in plants without the need for external power input.^102–107 During this process, semiconductor photocatalysts absorb sunlight to generate high-energy electrons, which can drive the conversion of CO₂ into organic compounds with high standard enthalpies of combustion, such as carbon monoxide, methanol, or methane, achieving conversion from solar to chemical energy.^108,109 Over recent decades, extensive efforts have been dedicated to the development and exploration of diverse semiconductor materials for CO₂ photocatalytic reduction, including metal oxides, oxynitrides, sulfides, and phosphides. Nevertheless, due to the inherently low electron affinity, pronounced chemical inertness, and exceptional structural stability of the CO₂ molecule, most photocatalysts face significant difficulties in efficiently interacting with it. Conventional semiconductors typically exhibit higher electron affinities than CO₂, giving rise to substantial thermodynamic barriers for CO₂ reduction, consequently diminishing the efficiency of photogenerated electrons in driving the reduction process.^110–112 Furthermore, due to variations in high-energy electron transfer mechanisms, CO₂ reduction can occur through multiple pathways, resulting in the formation of diverse products when single-component catalysts are employed. This diversity of reaction products not only increases the complexity of the catalytic system but also presents significant challenges in subsequent separation and purification steps, ultimately constraining the overall efficiency and feasibility of the reaction process.^113–115 Hence, achieving highly efficient and selective conversion of CO₂ into high-value-added fuel molecules remains a critical goal in the development of practical photocatalytic CO₂ reduction systems.

Photocatalytic CO₂ reduction represents a promising strategy for harnessing solar energy to convert carbon dioxide into sustainable fuels such as methane (CH₄). Owing to its wide bandgap, superior photostability, and favorable band alignment, GaN has demonstrated considerable potential in the field of CO₂ photoreduction.^116–118 However, bare GaN catalysts typically exhibit limited product selectivity in CO₂ reduction, posing a challenge for the efficient formation of the desired CH₄ product. To promote high selectivity toward CH₄ in CO₂ reduction, strategies such as precise modulation of the GaN surface electronic structure, defect states, and band positions can effectively suppress competing reaction pathways (e.g., formation of CO or H₂), thereby enhancing CH₄ selectivity.^119,120 Meanwhile, leveraging the synergistic effects between GaN and cocatalysts (e.g., noble metals like Pt and Pd, or non-noble metals such as Cu, Ni, and metal oxides) can significantly enhance photogenerated electron transfer and the catalytic activity of surface active sites, reduce activation energy barriers, and further improve CH₄ selectivity.^121,122 Hence, the rational design of GaN architectures in concert with cocatalyst integration offers a viable and effective strategy for improving both the efficiency and selectivity of CO₂ photoreduction to CH₄, paving the way for advanced CO₂ conversion technologies.

GaN possesses a more negative conduction band minimum (CBM) compared to most metal oxides, endowing it with superior kinetic reduction capability, which is particularly advantageous for reducing thermodynamically stable CO₂ molecules.¹²³ Furthermore, GaN satisfies the thermodynamic criteria for CO₂ reduction to carbon monoxide (CO) and hydrocarbons such as CH₄ across a broad pH window, highlighting its strong adaptability in complex catalytic systems.^124,125 Fabricating vertically aligned GaN nanowires on silicon substrates can further improve photocatalytic performance. These nanowires expose nonpolar m-plane sidewalls, which favor active site accessibility and efficient charge carrier transport. Nitride nanowires grown on heterogeneous substrates (e.g., Si) exhibit minimal crystal defects such as threading dislocations, owing to efficient lateral strain relaxation and the lack of rigid epitaxial constraints at the nanowire–substrate interface. This architecture markedly suppresses nonradiative recombination, thereby improving the utilization efficiency of photogenerated carriers. Fig. 7(a) schematically depicts the electrochemical potential pathways involved in the reduction of CO₂ to CH₄ and CO. Group III-nitride materials (AlGaInN) offer a tunable bandgap range of approximately 0.65–1.66 eV, enabling absorption across a broad spectrum of solar radiation. However, in GaN, photogenerated conduction band electrons may transfer to multiple adsorbed CO₂ intermediates, initiating parallel reduction pathways and leading to reduced product selectivity. To overcome this limitation, introducing cocatalysts that govern reaction selectivity has emerged as a crucial strategy.¹²⁶ For instance, Rh/Cr₂O₃ core–shell cocatalysts markedly enhance CH₄ evolution while reducing CO generation by nearly an order of magnitude. Fig. 7(b) illustrates the photocatalytic reduction pathway of CO₂ on GaN nanowires modified with Rh/Cr₂O₃ and Pt. This finding highlights the crucial role of such cocatalysts in directing electron transfer pathways and tuning product selectivity. Moreover, decorating the lateral m-plane surfaces of GaN nanowires with Pt nanoparticles can substantially boost the CO₂ photoreduction rate toward CH₄.¹²⁷ This is mainly attributed to the excellent electron trapping ability and catalytic activity of Pt, which facilitates multi-electron transfer processes and enhances the selective formation of CH₄.

CO₂ photoreduction was performed on both pristine GaN nanowires and samples surface-modified with Rh/Cr₂O₃ nanoparticles, with CO and CH₄ identified as the primary products.^128,129 As illustrated in Fig. 7(c), CH₄ evolution rates improved from 1.3 μmol g_cat⁻¹ h⁻¹ for unmodified GaN to 3.5 μmol g_cat⁻¹ h⁻¹ upon Rh/Cr₂O₃ modification, primarily due to enhanced CO₂ adsorption and hydrogenation capabilities of the cocatalyst. Fig. 7(d) shows that over a 24-hour period, pristine GaN generated a substantial amount of CO (∼1130 μmol g_cat⁻¹), whereas CO production was drastically reduced to ∼120 μmol g_cat⁻¹ in the Rh/Cr₂O₃-modified sample, evidencing a significant enhancement in CH₄ selectivity. Notably, CO evolution in the modified sample was suppressed beyond the initial 2 hours, indicating efficient capture of photogenerated electrons by Rh/Cr₂O₃, which in turn suppressed CO₂ reduction on unmodified sites. As shown in Fig. 7(e), CH₄ production on Pt-modified GaN nanowires reached ∼14.8 μmol g_cat⁻¹ h⁻¹ over 24 hours, representing nearly an order of magnitude increase compared to bare GaN. In contrast, Pt nanoparticle decoration had little effect on CO evolution, as evidenced by the inset in Fig. 7(e).

In conclusion, GaN nanowires present a compelling and efficient platform for the photoreduction of CO₂ into value-added fuels. The incorporation of Rh/Cr₂O₃ core–shell nanoparticles induces strong interfacial synergy with GaN nanowires, markedly improving the selectivity toward CH₄ in CO₂ photoreduction. This integrated catalytic system offers a robust foundation and technological basis for advancing selective and efficient CO₂ conversion toward practical fuel synthesis.

3.3. Photocatalytic N₂ fixation

GaN-based photocatalysts have demonstrated distinct potential in artificial nitrogen fixation, emerging as a promising alternative to the energy-intensive Haber–Bosch process. GaN combines a wide bandgap with remarkable chemical stability, and its conduction band lies above the nitrogen reduction potential, allowing photogenerated electrons to effectively reduce N₂ to NH₃ under light irradiation.^130–132 The built-in polarization field and facet-dependent effects of GaN further facilitate efficient spatial separation of charge carriers, suppressing recombination and enhancing the overall photocatalytic performance.^133,134 Engineering GaN into nanostructures such as nanowires or porous frameworks significantly increases surface-active sites, thereby enhancing the adsorption and activation of N₂ molecules.¹³⁵ Moreover, surface engineering via nitrogen vacancies or transition metal doping (e.g., Fe, Mo) effectively lowers the activation barrier for N–N bond cleavage, enabling more efficient electron transfer to the nitrogen molecule.¹³⁶ Experimental results confirm that GaN-based systems enable sustainable NH₃ generation under ambient conditions, featuring high photostability and reusability, thereby opening new avenues for green, efficient artificial nitrogen fixation technologies.

Mi et al. devised a robust and efficient approach for visible-light-driven nitrogen reduction by anchoring dense, ultrasmall Ru clusters onto GaN nanowires.¹³⁷ To enable visible-light absorption, indium was incorporated to narrow the GaN bandgap, extending its photoresponse into the visible region. InGaN/GaN nanowire arrays were grown on silicon substrates via MBE (Fig. 8(a)), and high-resolution STEM-EDXS analyses revealed the formation of five discrete InGaN segments along the nanowire axis, which effectively mitigated indium phase separation (Fig. 8(b)). Given the higher work function of Ru compared to n-type GaN, upward band bending at the interface formed a Schottky barrier, as shown in Fig. 8(c) which served as an efficient trap for photogenerated electrons under illumination.¹³⁸ This irreversible electron capture significantly suppressed charge recombination, thereby enhancing photocatalytic activity.¹³⁹

To further enhance charge carrier extraction and provide additional active sites for nitrogen activation, metallic Ru cocatalysts were deposited onto the surface of GaN nanowires. As shown in Fig. 8(d), the incorporation of Ru significantly improved the catalytic efficiency. The NH₃ production rate of Ru@n-GaN nanowires increased with increasing Ru loading, reaching a maximum at 5 wt%. When the Ru content exceeded this threshold, catalytic activity declined, primarily due to the reduced atomic utilization efficiency resulting from the aggregation of Ru clusters.¹⁴⁰ To investigate the nature of the catalytic active centers, Ru was loaded onto n-GaN nanowires by thermal decomposition of RuCl₃, yielding Ru*@n-GaN samples. Additionally, another type of catalyst was prepared using Ru₃(CO)₁₂ as the Ru precursor. Comparative experiments revealed no significant improvement in catalytic activity with Ru₃(CO)₁₂ (Fig. 8(e)), suggesting that the physical state of Ru plays a critical role in determining catalytic performance. As illustrated in Fig. 8(f), the InGaN nanowires loaded with 5 wt% Ru exhibited excellent catalytic performance, achieving an NH₃ production rate of 2400 μmol h⁻¹ g⁻¹. Under ambient conditions, the NH₃ yield of Ru@n-GaN was approximately five times higher than that of the unmodified sample, with the NH₃ concentration peaking after 24–25 hours (inset of Fig. 8(f)). Reusability tests demonstrated that the Ru@n-GaN catalyst retained its catalytic performance over eight consecutive cycles, indicating robust stability and recyclability.¹⁴¹

This study presents a visible-light-driven InGaN/GaN nanowire-Ru catalyst system NH₃, offering an efficient and stable strategy for photocatalytic N₂ fixation.

3.4. Photocatalytic degradation of pollutants

GaN-based photocatalysts have garnered significant interest for environmental pollutant degradation, owing to their wide bandgap, excellent chemical stability, and pronounced oxidative potential. Upon light excitation, GaN efficiently generates electron–hole pairs; the photogenerated holes exhibit strong oxidizing power capable of initiating direct or indirect degradation of organic pollutants into benign end-products such as CO₂ and H₂O.^142–144 In addition, rational design of nanostructures (such as nanowires or porous architectures) and surface defect engineering can substantially increase surface active site density and promote charge carrier separation, leading to enhanced pollutant degradation kinetics and mineralization efficiency.^145–148 Moreover, integrating cocatalysts such as Ag, Pt, or TiO₂ facilitates efficient photogenerated electron transfer and suppresses recombination, thereby accelerating the oxidative degradation pathways.^149–151 Consequently, GaN-based photocatalytic systems demonstrate outstanding performance in pollutant degradation and offer considerable potential for broad environmental remediation applications.

Considering the bandgap energies and band positions of the components, a type-II charge transfer pathway for the 3Co/0.3ZnIn₂S₄/GaN heterostructure during tetracycline degradation was constructed, as shown in Fig. 9(a).¹⁵² Upon visible-light exposure, ZnIn₂S₄ and GaN are both excited, leading to the formation of photogenerated electron–hole pairs. Due to the formation of a type-II heterojunction, electrons transfer from the conduction band of ZnIn₂S₄ to that of GaN, while holes migrate from the valence band of GaN to ZnIn₂S₄, resulting in spatial separation of charge carriers and significantly suppressing their recombination. Additionally, cobalt doping introduces favorable localized states within ZnIn₂S₄, which enhance electron transfer dynamics, further promoting charge separation and boosting the overall photocatalytic performance.^153,154 The conduction band potentials of ZnIn₂S₄ and GaN are sufficiently negative to reduce O₂ into *O₂⁻ radicals, which can subsequently form oxidative intermediates like H₂O₂. In contrast, their valence band positions are not positive enough to directly oxidize H₂O into *OH. Importantly, the valence band of GaN valence band is sufficiently positive to oxidize OH⁻ into *OH radicals, suggesting that *OH is most likely produced via a multistep process involving *O₂⁻ intermediates. Based on the analysis of active species, the contribution order to tetracycline degradation is h⁺ > *O₂⁻ > *OH, with photogenerated holes (h⁺) serving as the primary oxidative species driving the reaction.

Photoelectrochemical (PEC) measurements further confirmed the superior capability of the 3Co/0.3ZnIn₂S₄/GaN heterostructure in facilitating photogenerated charge carrier excitation and transport. As shown in Fig. 9(b), the GaN/sapphire electrode produced a stable yet minimal photocurrent under light irradiation, suggesting limited efficiency in charge carrier separation. In contrast, the photocurrent of 0.3ZnIn₂S₄/GaN increased significantly to 0.1 μA, approximately five times higher than that of GaN, demonstrating the pronounced enhancement of carrier separation and transport induced by ZnIn₂S₄. Nevertheless, the ZnIn₂S₄ component, with its small bandgap and nanostructured morphology, displayed a pronounced decline in photocurrent over time, indicating the persistence of rapid carrier recombination.¹⁵⁵ Upon cobalt doping, the 3Co/0.3ZnIn₂S₄/GaN sample displayed a further elevated initial photocurrent, underscoring the key role of Co²⁺ in enhancing charge separation, in line with its superior photocatalytic degradation efficiency. Furthermore, the practical applicability of 3Co/0.3ZnIn₂S₄/GaN was assessed in different real-water environments, namely distilled water, tap water, and actual pharmaceutical wastewater, as illustrated in Fig. 9(c). In tap water, the degradation efficiency of tetracycline reached 85%, outperforming the other systems, likely due to synergistic effects from coexisting ions. In actual pharmaceutical wastewater, despite the presence of a complex background matrix, the system still achieved 72% degradation efficiency, demonstrating strong promise for real-world applications.¹⁵⁶ The decline in efficiency is primarily attributed to the elevated concentrations of total dissolved solids and coexisting organic compounds in the wastewater, which likely compete with tetracycline for active radical species, thereby hindering the degradation process.^157,158

It is worth noting that this study is the first to systematically report the degradation behavior of tetracycline antibiotics (represented by tetracycline hydrochloride) using GaN-based photocatalysts in various real-water environments, providing both theoretical and experimental support for their practical environmental remediation applications. The stability and reusability of photocatalysts are key factors for practical application. However, the efficient recovery of photocatalysts in aqueous systems remains a challenge. Traditional recovery methods such as centrifugation and filtration are time-consuming and costly, making them unsuitable for large-scale engineering applications.^159,160 Recently, magnetically separable photocatalysts have been proposed as a promising alternative strategy, enabling rapid and efficient catalyst separation in water.^161,162 In this study, Co-doped ZnIn₂S₄ was immobilized on an inert GaN/sapphire substrate, which not only improved structural stability but also provided an effective strategy for catalyst recyclability. Cyclic experiments revealed that the 3Co/0.3ZnIn₂S₄/GaN system maintained approximately 70% tetracycline degradation efficiency after five successive cycles (Fig. 9(d)), demonstrating excellent long-term stability and reusability. Overall, the heterostructure exhibits not only excellent visible-light responsiveness but also structural robustness and recoverability, showing great potential for application in complex water environments.

3.5. Photocatalytic organic transformation

GaN-based photocatalysts have demonstrated outstanding capabilities in organic transformations, making them highly suitable for green and environmentally benign synthetic strategies. Due to its wide bandgap, GaN can be effectively photoactivated under UV or high-energy visible light to produce electron–hole pairs, where the strongly oxidizing holes are capable of activating C–H and CC bonds, thereby driving selective oxidation or coupling processes.^163–165 GaN has been employed as a crucial catalytic platform in diverse organic reactions, including alcohol oxidation, alkane functionalization, amine oxidation, and aromatization processes.¹⁶⁶ Moreover, tuning crystal facets of GaN, engineering surface defects, or constructing heterojunctions (e.g., with InGaN or ZnO) can further enhance its light absorption and charge separation efficiency, thereby improving catalytic rate and selectivity. Additionally, the incorporation of metal or non-metal cocatalysts (such as Cu, Co, or N dopants) can tailor the surface of GaN electronic structure and active sites, providing an optimized microenvironment for targeted organic reaction pathways. Consequently, GaN photocatalysis exhibits substantial potential in driving efficient and selective organic transformations, offering new paradigms for green synthetic chemistry and sustainable reaction systems.

Ethylene is a key raw material in the chemical industry, primarily used in the production of polymers and a variety of chemicals.^167–169 Currently, ethylene is mainly produced via steam cracking of naphtha and liquefied petroleum gas, which is energy-intensive and generates high carbon emissions, falling short of sustainability goals.^170–172 In contrast, bioethanol can be produced in large quantities from renewable resources such as sugarcane, starch, and lignocellulose via fermentation. It is currently used primarily as a fuel additive, and urgently needs to be directed toward higher-value applications.^173,174 Owing to structural similarity, ethanol can be converted to ethylene through dehydration. However, conventional dehydration processes typically require strong acids or bases, raising environmental concerns. Photocatalysis, as a green and solar-driven strategy, has shown great potential in biomass conversion. In recent years, photocatalytic conversion of ethanol to ethylene has gained attention. However, the high stability of C–C and C–O bonds, along with the poor selectivity of photogenerated reactive species (e.g., *OH, *O₂⁻), makes it challenging to achieve directional conversion.^175–177 Therefore, the development of efficient and highly selective photocatalyst systems is urgently needed. One-dimensional vertically aligned gallium nitride nanowires (GaN NWs) have exhibited excellent performance in photocatalysis. When grown on silicon substrates, they enhance light absorption and reduce scattering, while offering high electron mobility, low defect density, and short carrier diffusion paths, all of which contribute to efficient charge separation. Their large specific surface area and tunable surface polarity provide favorable conditions for anchoring active sites and modulating electronic structures.

Fig. 10(a) illustrates a schematic of ethanol photocatalytic dehydration to ethylene over surface-hydrogenated CrMnOx coupled with a GaN nanowire (GaN@CMO-H) nanostructure.¹⁷⁸ Under visible-light irradiation, this structure facilitates the conversion of biomass-derived ethanol to ethylene by effectively mediating the interaction between photogenerated charge carriers and ethanol.^179,180 To gain deeper insight into the reaction pathway of ethanol dehydration, density functional theory (DFT) was employed to systematically analyze the underlying molecular mechanism. First, the adsorption behavior of ethanol on different catalytic surfaces was investigated. As shown in Fig. 10(b), ethanol exhibits a strong adsorption energy of −1.252 eV on bare GaN, indicating favorable surface interaction. Upon the introduction of surface-hydrogenated CrMnO_x (CMO-H), the adsorption energy increases to −1.064 eV, indicating a weakened interaction between ethanol and the catalyst. Furthermore, GaN@CMO obtained by annealing (removal of surface hydrogen) exhibits stronger ethanol adsorption (−1.557 eV), which may not be kinetically favorable for subsequent reaction steps. Subsequently, the Gibbs free energy profile for ethanol dehydration to ethylene was constructed. As shown in Fig. 10(c), on bare GaN, the reaction barrier for *C₂H₅OH → *C₂H₅ + *OH is 0.314 eV, while the rate-determining step *C₂H₅ → *C₂H₄ + *H has a barrier of 0.857 eV, indicating the reaction is limited by a high energy barrier. In contrast, the introduction of CMO-H or CMO significantly alters the reaction pathway. Notably, on the GaN@CMO-H surface, surface hydrogen participates in the direct conversion of ethanol-derived OH via the pathway: GaN@CMO-H + *OH + C₂H₅ → GaN@CMO + H₂O + C₂H₅*, which is distinct from the mechanism on GaN or GaN@CMO (i.e., *C₂H₅ + *OH → *C₂H₄ + *H + *OH). This mechanistic shift facilitates H₂O formation and indirectly promotes ethylene production. The dehydrogenation site is replenished via *C₂H₅, ultimately releasing C₂H₄. Notably, in the GaN@CMO-H system, the rate-limiting step switches from *C₂H₄ desorption to *H₂O desorption, with the corresponding energy reduced from 0.777 eV (GaN@CMO) to 0.643 eV. Additionally, as shown in Fig. 10(d), the formation of the key intermediate *H₂O requires only 0.288 eV on GaN@CMO-H, significantly lower than on GaN@CMO (0.606 eV) and bare GaN (0.857 eV). The bimetallic coupling of Cr and Mn modulates the adsorption strength of key intermediates, with catalytic activity following the order: GaN@CMO-H > GaN@CMO > GaN, consistent with DFT results. In summary, both experimental and theoretical findings confirm that the introduction of surface hydrogen on GaN@CMO-H not only modifies the ethanol dehydration pathway but also reduces energy barriers and enhances overall catalytic efficiency.^181,182 Surface hydrogen plays a key role in modulating the reaction pathway and facilitating the photocatalytic conversion of ethanol to C₂H₄ (as depicted in Fig. 10(a)).

In this study, for the first time, surface-hydrogenated binary Cr–Mn oxides are coupled with GaN nanowires grown on silicon substrates to construct an efficient light-driven ethanol dehydration system, enabling sustainable conversion of bioethanol to ethylene. This system provides a new route for utilizing solar energy to convert biomass-derived feedstocks into key platform chemicals such as ethylene, showing great potential for replacing fossil resources in green chemical manufacturing.

4. Conclusions and perspectives

GaN is a highly adaptable wide-bandgap semiconductor that has exhibited significant promise in a broad spectrum of catalytic applications. Owing to its inherent properties, which include excellent chemical and thermal stability, adjustable electronic structures, and pronounced redox activity, GaN has contributed to significant advances in hydrogen evolution, CO₂ reduction, N₂ fixation, pollutant degradation, and energy-efficient organic transformations. Together, these advances underscore the critical role of GaN in addressing pressing global challenges related to energy sustainability and environmental protection. Despite substantial progress, major barriers still limit the full realization of GaN's catalytic capabilities, and addressing these limitations requires coordinated interdisciplinary approaches to translate laboratory research into scalable practical solutions.

The limitations of GaN-based systems are primarily attributed to their confinement of light absorption to the ultraviolet region, the rapid recombination of photogenerated carriers, the elevated costs associated with scalable synthesis, and an inadequate mechanistic understanding of selectivity within intricate reaction pathways. These challenges point to the urgent need for novel approaches that enhance both material characteristics and reaction system design. For example, bandgap tuning through alloying can expand light absorption into the visible region, while advanced in situ techniques such as X-ray absorption fine structure and diffuse reflectance infrared Fourier transform spectroscopy are essential for probing real-time surface dynamics and identifying transient intermediates. In addition, incorporating artificial intelligence for high-throughput screening and employing machine learning in catalyst design holds great potential to accelerate the development of optimized GaN-based composites with improved performance and durability.

Looking ahead, the advancement of GaN catalysis will be driven by the convergence of diverse scientific disciplines through synergistic collaboration. Achieving scalability will require close collaboration among materials scientists, chemical engineers, and computational theorists to refine architectures such as Z-scheme heterojunctions and to design flow reactors that meet industrial requirements. In parallel, the exploration of surface defect modulation, precision doping techniques, and hybrid frameworks including GaN-MOFs or carbon-integrated architectures is essential for suppressing charge carrier recombination and improving catalytic selectivity. Through the promotion of cross-disciplinary innovation and a focus on practical relevance, GaN-based catalytic systems have the potential to initiate a transformative shift toward sustainable energy conversion and environmental management, bridging the divide between experimental discovery and technological implementation.

Author contributions

Kun Wang: writing – review draft, resources. Yunchao Lei: recent progress analysis. Zefei Wu: investigation. Mengyang Zhang: writing – review & editing challenges and future perspective section. Ting Zhi: writing – review & editing, supervision, project administration. Longlu Wang: writing – review & editing, project administration, supervision.

Conflicts of interest

There are no conflicts to declare.

Data availability

No primary research results, software or code have been included and no new data were generated or analysed as part of this review.

Acknowledgements

This work was financially supported by the Natural Science Foundation of China (51902101), the Natural Science Foundation of Jiangsu Province (BK20201381), the Science Foundation of Nanjing University of Posts and Telecommunications (NY219144 and NY221046), and the National College Student Innovation and Entrepreneurship Training Program (202310293010Z).

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