Mechanism Of Hydrogen Production Research Articles

Insight into the effect of CeO2 morphology on catalytic performance for steam reforming of glycerol

Shape-specific CeO2 nanocrystals (spheres, rods, cubes and nanoparticles) with well-defined crystal facets were successfully synthesized and used as the support to synthesize series Ni/CeO2. Ni/CeO2 was employed as the model catalysts to study the structure dependent behavior and reaction mechanism for hydrogen production from glycerol steam reforming (GSR). The metal-support interaction was finely tuned by altering the morphology of CeO2 support, which in turn affected the exposed specific surface area of nickel and oxygen vacancy concentration. The relationship between exposed surface area of active nickel as well as surface oxygen vacancies and catalytic performance was studied. Ni/CeO2-S with the mainly exposed (111) type planes obtained the strongest metal-support interaction. Electron effects due to the strong metal-support between nickel and cerium dioxide facilitated the formation of readily reducible nickel species (Niδ+). High nickel reduction and nickel dispersion contributed to the maximum active nickel exposure surface area, thus Ni/CeO2-S showed exceptional glycerol conversion. Meanwhile, the strong Ni-CeO2 interaction resulting in abundant oxygen vacancies that facilitated the dissociation of water to produce hydrogen, thus possessing a high H2 yield. Conversely, Ni/CeO2-NR and Ni/CeO2-NC have lower exposure areas and oxygen vacancy concentrations due to the different exposed crystal planes, and therefore have relatively poor catalytic activity. Moreover, the strong oxygen storage-release ability (CO-OSC-OSCC) promoted the oxidation of carbon deposition on Ni/CeO2-S. Additionally, carbon deposition was mainly the filamentous carbon growing towards the periphery, hence, Ni/CeO2-S obtained up to 25-h catalytic stability. The study of the regulatory role of Ni-CeO2 interaction on catalytic behavior can offer worthwhile direction for designing high-efficiency GSR catalysts.

Chalcogenides and Chalcogenide-Based Heterostructures as Photocatalysts for Water Splitting

Chalcogenides are essential in the conversion of solar energy into hydrogen fuel due to their narrow band gap energy. Hydrogen fuel could resolve future energy crises by substituting carbon fuels owing to zero-emission carbon-free gas and its eco-friendliness. The fabrication of different metal chalcogenide-based photocatalysts with enhanced photocatalytic water splitting have been summarized in this review. Different modifications of these chalcogenides, including coupling with another semiconductor, metal loading, and doping, are fabricated with different synthetic routes that can remarkably improve the photo-exciton separation and have been extensively investigated for photocatalytic hydrogen generation. In this direction, this review is undertaken to provide an overview of the enhanced photocatalytic performance of the binary and ternary chalcogenide heterostructures and their mechanisms for hydrogen production under irradiation of light.

(Digital Presentation) Cathodic Exfoliation of Few-Layer Tellurium As Electrocatalyst Support for Hydrogen Evolution

Few-layer tellurium represents the two-dimensional (2D) form of tellurium crystal with the majority of the Te atoms exposed on its surface. Recent studies demonstrated that 2D Te has good environmental stability and high charge carrier mobility, making it suitable electrocatalyst support to host active sites and assist electron transfer between the electrode and the sites [1]. Yet, its mass production for electrocatalysis application remains challenging.In this study, we present a simple cathodic exfoliation method to exfoliate commercially available Te crystal directly into few-layer tellurium with exceptionally high yield [2] (see Figure 1A). Using alkaline aqueous electrolyte (1.0 M KOH), Te nanosheets with the thickness of 7~10 nm and lateral size of 1~4 µm were produced at an applied potential of −0.42 V (vs. RHE). Combining in situ Raman spectroscopy and ex situcharacterization results, we were able to reveal the exfoliation mechanism, where the in situ generated ditelluride (Te2 2−) anions on the nanosheets played the critical role of separating nanosheets from the bulk crystal (see Figure 1B).At the presence of transition metal ions in the electrolyte, such as Pt2+ and Ni2+, simultaneous surface doping of Te nanosheets was enabled by the interaction between Te2 2− anions and metal ions, producing Pt/Ni-doped Te with tunable doping level. Such doped nanosheets exhibited high stability and hydrogen evolution reaction (HER) activity. Particularly at high potential, Pt-doped Te nanosheets outperformed both polycrystalline Pt and commercial Pt/C catalysts (see Figure 1C). We suggested a collaborative hydrogen production mechanism via Volmer–Heyrovsky pathway to justify such unusual activity. In short, at HER conditions, the surface Te atoms of Pt-doped Te nanosheets are reduced to Te2 2− anions. Such species can help attract protons and assist their transfer to adjacent Pt atoms, where the protons are reduced to form hydrogen (see Figure 1D). Figure 1 (A) Experimental setup and photos of the electrochemical exfoliation of Te crystal; (B) Exfoliation mechanism; (C) HER performance and relative energy of Pt-doped Te with various doping levels; (D) Collaborative HER mechanism. Reference: Shi, Z.; Cao, R.; Khan, K.; Tareen, A. K.; Liu, X.; Liang, W.; Zhang, Y.; Ma, C.; Guo, Z.; Luo, X.; Zhang, H., Nano-Micro Lett. 2020, 12 (1), 99. Zheng, W.; Li, Y.; Liu, M.; Lee, L. Y. S., Small 2021, 17 (18), e2007768. Figure 1

1 D CeO2/g-C3N4 type II heterojunction for visible-light-driven photocatalytic hydrogen evolution

• One-dimensional hollow tubular CeO 2 /g-C 3 N 4 heterojunctions were prepared by electrospinning and vapor deposition. • The recombination of photogenerated electrons and holes is effectively inhibited by one-dimensional hollow tubular morphology and binary heterojunction structure. • CeO 2 /g-C 3 N 4 improves the photocatalytic hydrogen production performance and has good cycle stability. Hydrogen production by photocatalytic water splitting for hydrogen production using solar energy is considered to a relatively green technology. In this study, we prepared one-dimensional hollow tubular CeO 2 /g-C 3 N 4 materials with heterojunctions by electrospinning and vapor deposition. When the amount of melamine used in vapor deposition was 1.5 g, CeO 2 /g-C 3 N 4 composites showed the strongest photocatalytic hydrogen production activity (229.75 μmolg −1 ·h −1 ). Meanwhile, the CeO 2 /g-C 3 N 4 -1.5 g composite has good photocatalytic hydrogen production stability, and at the end of this paper, we propose a possible photocatalytic hydrogen production mechanism. It was well known that the improvement of photocatalytic hydrogen production activity was mainly on account of the regulation of its one-dimensional morphology and the formation of heterostructures. Which it significantly broadens the responsiveness of the material to visible light, promotes the separation of photogenerated electrons and holes, and improves the photocatalytic hydrogen production activity.

Partial phosphating of Ni-MOFs and Cu2S snowflakes form 2D/2D structure for efficiently improved photocatalytic hydrogen evolution

2D Cu2S snowflakes and 2D Ni-MOFs flakes were synthesized by hydrothermal method, and Ni-MOFs were calcined with sodium hypophosphite at 200 °C to form Ni-MOFs-P (Ni-MOFs/Ni2P). In the physical mixing process, since the -formation temperature of Cu2S is at 80 °C, the physical mixing temperature was controlled at 80 °C, which is advantageous for achieving a close 2D/2D contact. The results showed that 15 vol% TEOA with pH = 10 was used as sacrificent reagent under 5 W LED simulated visible light. 20 mg of EY was used as a photosensitizer. CNP60 had the best hydrogen evolution performance within 5 h, which was 3122.76 μmol g−1 h−1. The hydrogen evolution rate of CNP60 is 8.72 fold, 3.37 fold, and 91.85 fold faster than that of Ni-MOFs, Ni-MOFs-P, and Cu2S, respectively. Ni-MOFs phosphating and Cu2S loading can reduce the photocatalyst's photogenerated electron and hole recombination efficiency. This significant improvement was achieved through XRD, SEM, TEM, XPS, UTV-Visible DRS, transient photocurrent, steady-state fluorescence, short fluorescence, related substance reporting studies, radical hydroxyl trapping, and more. The results show that the 2D/2D assembled CNP can effectively enhance the ability to reduce H∗, and a possible photocatalytic hydrogen production mechanism is proposed.

Mechanism research on hydrogen production from catalytic pyrolysis of waste tire rubber

Waste tires are currently disposed of through various approaches such as landfill and incineration, which not only causes environmental pollution, but also lead to the wastage of resources. As an important type of solid waste, tire rubber has a high carbon-to-hydrogen ratio, which makes it a good material for hydrogen production from pyrolysis. In this study, molecular dynamics simulations combined with experimental methods are used to explore the mechanism of hydrogen production from the catalytic pyrolysis (CP) of waste tire rubber (WTR) over Ni, ZSM-5 and Ni/ZSM-5. The simulation results show that the three catalysts potentially promote the release of hydrogen radicals from monomers and facilitate attack by H· radicals to generate hydrogen. Compared with ZSM-5 and Ni, the Ni/ZSM-5 catalyst exerts better catalytic effects, leading to higher contents of produced H2 and hydrocarbons. In the low-temperature stage, the long chain cracks into monomer compounds, which mainly include isoprene, styrene, and 1,3-butadiene. Meanwhile, in the high-temperature stage, free radicals attack monomers to generate small molecules. The main gas products from the catalytic pyrolysis of waste tire rubber are hydrogen, methane, and ethylene. The use of all three catalysts leads to a low final catalytic pyrolysis temperature, high catalytic pyrolysis rate, and excellent catalytic effect. This work aims to provide a deeper understanding of the reaction thermodynamics and kinetics for the formation mechanisms of gaseous products, primarily hydrogen.

A review in redressing challenges to produce sustainable hydrogen from microalgae for aviation industry

The global depletion of fossil fuel reserves and associated environmental crisis have led researchers to explore microalgal biomass which has been proven could be a promising potential as a renewable energy feedstock. Biofuels such as biodiesel, bioethanol and hydrogen can be produced from microalgae. Indeed, microalgae are best employed for hydrogen generation because the microalgal cells have high growth rate, can grow in diverse habitats and non-arable lands, can solve the fuel versus food conflicts as well as can capture and assimilate the atmospheric carbon dioxide. Hydrogen that is produced from microalgae is a clean and sustainable option to replace or complement the fossil fuel demands. The combustion of hydrogen produces only water and no greenhouse gases emission which will assuage the untoward effect on the environment. Moreover, it can also be used directly to generate electricity in fuel cells and engines. Another sector that is looking into hydrogen as a replacement for fossil fuels, is transportation inclusive of the aviation industry. The use of hydrogen as an energy carrier in airplanes offers several advantages, the burning of hydrogen in the jet engines would produce water vapour which will eliminate carbon-related emissions. However, this also comes with limitations such as new designs and larger tanks for hydrogen storage. Besides, the mechanisms of hydrogen production from microalgae are also sporadic and not well documented systematically, pre-empting researchers from exploring this new energy source inclusively. The factors affecting the microalgal hydrogen production are as well essential, but still poorly conceived, leading to the low outputs in terms of hydrogen yields from microalgae. Accordingly, this article reviews various mechanisms and methods employed for producing hydrogen from microalgae as well as the pre-treatment procedures for enhancing the rates of hydrogen production from microalgae. Furthermore, the enhancement of hydrogen yields through state-of-the-art techniques and genetic engineering the microalgal strains are also unveiled to materialize the hydrogen production at an industrial scale. This review intents to shift the paradigm from typical hydrocarbon biofuels to green hydrogen adoption, hastening the carbon neutrality target that benefits the natural environment the most.

Molecular mechanism of hydrogen production in membrane-bound hydrogenase

Molecular mechanism of hydrogen production in membrane-bound hydrogenase

Fabrication of visible-light-driven bimetallic MOF-derived Ag/NiOx/N-TiO2: Photocatalytic hydrogen production mechanism and methanol transformation pathway

A novel bimetallic metal–organic framework (MOF)-derived Ag/NiOx/N-TiO2 photocatalyst with a Z-scheme system was successfully synthesized for photocatalytic hydrogen production. The as-prepared photocatalysts were characterized using X-ray diffraction, scanning electron microscopy, transmission electron microscope, X-ray photoelectron spectroscopy, UV–vis spectroscopy, photoluminescence, and photoelectrochemical techniques. Compared to N-TiO2, the Ag/NiOx/N-TiO2 composite material with a wider light absorption range exhibited outstanding photocatalytic hydrogen production using methanol as a sacrificial agent. The optimum Ag/NiOx ratio (5 wt%) results in a hydrogen production rate of 1240 μmol·g−1·h−1 in a 50 v/v% methanol solution. According to the results of the durability test, the synthesized photocatalyst demonstrates good stability. Consequently, a possible mechanism of the photocatalysts and the transformation pathway of methanol have been reported. The Z-scheme system of NiOx and N-TiO2 can effectively separate the electron-hole pairs. The surface plasmon resonance effect of Ag0 enhanced the visible light response. This study provides a valuable reference for the synthesis of MOF-derived photocatalytic technologies and the mechanism of rapid and efficient hydrogen production.

Electrochemical Behavior of Mono‐Substituted [FeFe]‐Hydrogenase H‐Cluster Mimic Mediated by Stannylated Dithiolato Ligand

AbstractIn this research work we present the synthesis and characterization of asymmetrical [FeFe]‐hydrogenase mimic, [Fe2(CO)5P(OMe)3{μ‐(SCH2)2SnPh2}] (2), obtained from replacing one of the CO ligands of the parent hexacarbonyl complex [Fe2(CO)6{μ‐(SCH2)2SnPh2}] (1) with the monodentate phosphite P(OMe)3. The molecular structure of complex 2 was confirmed by X‐ray diffraction analysis. Moreover, the electrochemistry of complexes 1 and 2 was investigated to explore the influence of the steric bulk of the Ph‐ring at the bridgehead Sn atom with the nearby P(OMe)3 ligand. In addition, both complexes show their potentials toward hydrogen formation in the presence of weak acid, such as acetic acid (AcOH), suggesting an ECEC (E=electron transfer, C=chemical process) mechanism for hydrogen production.

Defect MoS2 and Ti3C2 nanosheets co-assisted CdS to enhance visible-light driven photocatalytic hydrogen production

The addition of a co-catalyst is one of the most effective ways to enhance the performance of CdS photocatalytic hydrogen production. In this work, ternary photocatalysts with Defect MoS2 and Ti3C2 acting synergistically on CdS are explored. The experimental results showed that the Defect MoS2/Ti3C2/CdS photocatalyst had excellent photocatalytic hydrogen production performance of 14.1 mmol h−1g−1, which was 18.5, 12.4, and 1.2 times higher than that of CdS, Ti3C2/CdS and Defect MoS2/CdS, respectively. Defect MoS2 and Ti3C2 synergistically interact with CdS and form heterojunctions, which improve the carrier separation efficiency and effectively suppress the recombination of photogenerated carriers. A possible photocatalytic hydrogen production mechanism of Defect MoS2/Ti3C2/CdS is also proposed. The dual co-catalysts of Defect MoS2 and Ti3C2 demonstrated in this paper provide a feasible approach for the development of composite catalysts.

Analysis of several main hydrogen production technologies

With economic development, social progress, and population growth, mankind’s demand for energy increases. Fossil fuels such as coal, oil, and natural gas are accelerating consumption, and these fossil fuels are non-renewable, and their reserves are very limited. If we continue to use fossil fuels uncontrollably, it will inevitably cause acid rain and global warming. As a renewable energy source, hydrogen energy has the least environmental pollution, and hydrogen energy can be dispersed in large quantities and converted from renewable energy. At present, hydrogen production technology and cost are high. This article briefly explains the principles and advantages, and disadvantages of several hydrogen production technologies, etc., and the cost and work efficiency of various technologies. Studies have shown that biomass pyrolysis and photocatalytic hydrogen production have higher efficiency and lower cost, which can be used as future research directions. However, there are problems such as the unclear hydrogen production mechanism of biological pyrolysis and unstable solar energy. And its future research and development directions are discussed in more detail. The research on hydrogen production technology is to satisfy the requirements of national economic development and social development needs.

Facile formation of Mo-vacancy defective MoS2/CdS nanoparticles enhanced efficient hydrogen production

In this work, a novel Mo vacancy defective MoS2 loaded on CdS nanoparticles were obtained by a facile hydrothermal method. The photocatalytic performance of the prepared composites was evaluated from the perspective of decomposing water to produce H2. The experimental result showed that the release rate of H2 with defect MoS2/CdS composites is 11,750 μmol g−1h−1, which is 1.3 and 15.3 times higher than that of MoS2/CdS composites without defect (Mo) and pure CdS, respectively. The defective (Mo) vacancies formed on the MoS2 surface due to partly oxidized by potassium permanganate. The synergistic interaction of defect MoS2/CdS composites exhibited significant photocatalytic hydrogen production performance. The possible photocatalytic hydrogen production mechanism of the defect MoS2/CdS was suggested. This study provides a new way to prepare efficient hydrogen production photocatalysts based on defective metal vacancy.

Efficient photocatalytic hydrogen evolution through reverse hydrogen spillover on photoactivated copper-doped mesoporous titania spheres

Transition-metal-doped mesoporous TiO2 (M-mTiO2) spheres are highly desired for photocatalysis because of their large specific surface area and extended light absorption. Herein, a universal method is developed for the preparation of M-mTiO2 spheres and their photocatalytic mechanism is unveiled. Fe-mTiO2, Co-mTiO2, Ni-mTiO2, Cu-mTiO2 spheres are successfully prepared by the developed method. Among all M-mTiO2 samples, the Cu-mTiO2 catalyst exhibits reversible photoactivation phenomenon during photocatalysis. The photocatalytic hydrogen evolution rate on photoactivated Cu-mTiO2 can reach 3.31 mmol g−1 h−1, which is much higher than those of other M-mTiO2 and is 28.3 times of that of the mTiO2. Density functional theory (DFT) calculations reveal that the photoactivation of Cu-mTiO2 is associated with the facile formation of oxygen vacancies on Cu-mTiO2. The photoactivation induces the active site change and the light absorption increase of Cu-mTiO2. The active site change has the dominant role for the enhancement of photocatalytic performance. On the photoactivated Cu-mTiO2, the hydrogen production is through a reverse hydrogen spillover process. Our findings not only provide a universal method for the preparation of M-mTiO2 but also deepen the understanding about the photoactivation and the hydrogen production mechanism.

A novel dinuclear cobalt-bis(thiosemicarbazone) complex as a cocatalyst to enhance visible-light-driven H2 evolution on CdS nanorods and a mechanism discussion

Photocatalytic water splitting to produce hydrogen has gradually become a research hotspot in recent years, and molecular cocatalysts especially cobalt-based complexes as proton reduction cocatalysts have attracted wide attention due to their high activity and selectivity. In this study, CdS nanorods were employed as photosensitizers, and a novel dinuclear cobalt-bis(thiosemicarbazone) complex with definite structure was used as a cocatalyst to improve visible-light-driven hydrogen evolution. Under the optimum conditions, this noble metal-free system exhibited an average hydrogen evolution rate of 1045 μmol·h−1 in 8 h irradiation. This system could work for 24 h with a TON of 16,400, and the average apparent quantum yield of this system is ∼21% at 420 nm. On the basis of photoelectrochemical studies and electrochemical analysis, we proposed a possible mechanism for hydrogen production in this three-component system.

Pd single-atom decorated CdS nanocatalyst for highly efficient overall water splitting under simulated solar light

Solar-induced overall water splitting to produce hydrogen is inspiring towards energy sustainability, but it is also formidable due to its limited efficiency seriously hindering its scale up for practical application. CdS is an important transition metal sulfide with low-work-function. However, its photostability is often deteriorated due to photocorrosion influence. To overcome this issue, single-atom Pd was employed here to decorate CdS to form a CdS-Pd nanocatalyst through a simple and controllable photoinduced reduction strategy. The synergetic semiconductor (CdS)-metal (Pd) interaction promotes the fast bulk-to-surface electron migration, thereby the resultant CdS-Pd (3.83‰) nanocatalyst shows considerable structural stability and dramatically improved solar-induced HER activity in overall water splitting, about 110-fold higher than that of pristine CdS. Meanwhile, high apparent quantum yields (AQYs) of 4.47%/1.81% and 33.92%/27.49% were respectively achieved with this decorated nanocatalyst under the light of 420 nm/500 nm in absence and presence of scavenger, demonstrating the high-efficiency under broadband light illumination. Density functional theory (DFT) calculation supports that the easy formation of H* intermediates on the decorated nanocatalyst due to low energy barriers accounts for the internal promoted mechanism for hydrogen production. This study provides important insight to gain stable CdS-based photocatalysts for high-efficient hydrogen production by overall water splitting.

A novel cobalt complex of bptd and cobalt lactate complex to synergistically enhance photocatalytic HER activity and stability on CdS nanorods

A heterocycle 2,5-bis(2-pyridyl)-1,3,4-thiadiazole (bptd) as a polydentate reacts with CoCl2∙6H2O and NiCl2·6H2O to form two novel monomeric complexes, [Co(bptd)2Cl2]∙4H2O (1) and [Ni(bptd)2Cl2]∙4H2O (2). The complex 1 can act as electron cocatalyst to improve the rate of hydrogen evolution of CdS NRs under visible light irradiation. After the introduction of cobalt lactate complex as a hole cocatalyst, this noble-metal-free system exhibited a hydrogen evolution rate of 1123 ​μmol ​h−1, which is 12.2 times higher than that of pure CdS NRs. This system could work for 50 ​h with a TON of 7490, and the average AQY is 17% at 420 ​nm. Based on the results of experiments, the synergistic effect of complex 1 and cobalt lactate complex is proved and a possible mechanism for hydrogen production is proposed. This work may provide a reference for remedying the defects of faster carrier recombination and photocorrosion of CdS in heterogeneous environment.

A theoretical catalytic mechanism for methanol reforming in CeO2 vs Ni/CeO2 by energy transition states profiles

We present a theoretical study using Halgren-Lipscomb algorithm assisted by DFT + U to determine the catalytic mechanism for hydrogen production by steam reforming of methanol over CeO2 and Ni/CeO2 model catalytic surfaces. Our main goal is to describe the physical-chemical interaction between nickel with CeO2 matrix support and catalytic conversion mechanism in response to experimental evidence. The results from transition energy states in (111¯) and (11¯1¯) CeO2 surfaces, with and without nickel cluster, indicate that process is favored when metallic nickel is contained, however, exothermic energies in bare CeO2 supports prior suggestions ascribing the particular catalytic activity enhancement of Ni/CeO2 nanorod for methanol steam reforming due a synergistic effect of the CeO2 exposed planes of the nanorods and Ni clusters. Our aim is to provide key data for the improvement and enhancement, in terms of efficiency and viability, the current production of hydrogen by methanol steam reforming by Ni/CeO2 systems.

CdS nanorods supported copper-nickel hydroxide for hydrogen production under direct sunlight irradiation

A series of composite photocatalysts based on CdS nanorods decorated with Cu/Ni hydroxides were prepared via deposition precipitation method at room temperature (total metal loading ≈ 3 wt%). The performance of these photocatalysts was evaluated for H2 production through water dissociation reaction under direct sunlight. The 2.4Cu(OH)20.6Ni(OH)2/CdS photocatalyst with a total 3 wt% nominal metal cocatalyst loading demonstrated an excellent hydrogen production activity of ~20 mmol h−1g−1, that is 2 and 20 times greater than the benchmark Au/CdS and pristine CdS photocatalysts, respectively. Detailed analyses based on UV–Visible diffuse reflectance spectroscopy (DRS), X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), steady state photoluminescence (PL) and energy dispersive spectroscopy (EDS) suggested cocatalysts Cu/Ni hydroxides were transformed into their metallic states during photoreaction. Cu° was produced by the transfer of electrons due to the as available position of CdS conduction band (E°=0.61 V) to surface Cu(OH)2 nanoclusters (Cu(OH)2/Cu°, E°= 0.224 V) whereas Ni° was produced by the shift in conduction band level of CdS under continuous sunlight illumination (Ni(OH)2/Ni°, E°= 0.72 V). Based on these observations, the mechanism of hydrogen production from water splitting over Cu/Ni(hydroxides)-CdS was described.

Morphology Controllable Fabrication of Tungsten Oxide for Enhanced Photocatalytic Performance

Exploring the morphology-property relationship is an important role in addressing the mechanism of hydrogen production. In this work, WO3 photocatalysts with different morphology were prepared via a solvothermal method. Our first prepared porous WO3 with the exposed (100) crystal plane, the WO3 porous nano disk demonstrates a better photocatalytic activity, which is higher than the WO3 nanorod, WO3 nanoflower and WO3 nano block. Further characterizations indicate the WO3 porous nano disk exhibits high absorption capacity and active lattice structure. Meanwhile, with the introduction of non-noble metal Ni as the co-catalyst, the photocatalytic H2 evolution was enhanced. This work reveals the importance of regulating surface atomic configuration and catalytic active sites, opens a new avenue for the development of solar-driven water splitting.