Accelerated Charge Transfer Research Articles

S-Cu-FC/CuS modified GO carboxymethyl cellulose hydrogel for enhanced photocatalytic sterilization through homo-heterojunction interface accelerated charge transfer.

Charge transfer and separation play a critical role in the photocatalytic efficiency of photoresponsive materials and their subsequent applications. Herein, for the first time, we constructed a homo-heterostructured S-Cu-FC/CuS modified carboxymethyl cellulose (CMC) hydrogel doped with graphene oxide (GO) (S-Cu-FC/CuS/GO@CMC) through an in situ ionic complexation reaction, which exhibited enhanced photocatalytic performance under 808 nm near-infrared (NIR) light irradiation. On the one hand, photo-excited charges can rapidly transfer across the homo-heterojunction interface with copper atoms in S-Cu-FC/CuS as both donors and acceptors. On the other hand, the interface between GO and S-Cu-FC/CuS also favors the fast transfer of photogenerated charges. Hence, with the assistance of a photothermal effect, the enhanced photocatalytic performance of S-Cu-FC/CuS/GO endowed the hydrogel with robust sterilization ability for killing 99.5% S. aureus and 100.0% E. coli under 10 min NIR light irradiation. An in vivo test disclosed that this hydrogel could also accelerate the healing of bacteria-infected wounds.

Enhancing Low–Bias performance of n–type Cu2O photoanode for solar water splitting via simultaneously accelerated charge transfer kinetics at back contact and liquid junction

Poor low–bias PEC performance of state–of–the–art BiVO4, α–Fe2O3 and WO3 photoelectrodes widely used in tandem and/or parallel PEC/PV and/or PEC/PEC devices has been reported to largely limit the cell efficiency for self–biased solar water splitting. A breakthrough of such bottleneck is put forward in this contribution by employing n–Cu2O with advantageous band edge positions straddling the HER and OER redox potentials as an alternative photoanode. The ohmic Cu/n–Cu2O back contact facilitates the interfacial photoelectron transfer while the gradient distribution of the oxygen vacancies (Vo) close to the n–Cu2O/electrolyte junction promotes the photoholes injected into water, synergistically leading to an outstanding photocurrent density of 3.5 mA cm−2, an unprecedented photocurrent–to–O2 conversion efficiency exceeding 70%, and a record ABPE of 2% at an ultralow applied potential of ∼0.6 VRHE, among the highest performance and the lowest external bias of state–of–the–art metal–oxide–based photoanodes reported to date.

Electrolyte modification method induced atomic arrangement in FeOx/NF nanosheets for efficient overall water splitting.

To explore transition metal-based electrocatalysts with remarkable energy storage and conversion performance, the rational design and synthesis of electrodes with rich active sites and favorable electrical conductivity are crucial. Herein, using fluoroethylene carbonate (FEC) additive in electrochemical conversion reaction (electrolyte modification method) is proposed as an effective strategy to enhance the catalytic activity of FeOx/NF. The optimal sample FeOx/NF-Li-FEC1 shows optimized HER activity with remarkably low overpotential of 222 mV at a current density of 200 mA cm-2. By employing FeOx/NF-Li-FEC1 as bifunctional electrocatalysts, the overall water-splitting device reaches a current density of 10 mA cm-2 at a low cell voltage of 1.56 V. The outstanding performance is mainly attributed to the atomic arrangement to offer rich active sites as well as the evolved electronic structure and the thin SEI layer to accelerate charge transfer process. This study opens up a novel avenue to rationally design and synthesize low-cost and high-performance electrode materials for electrochemical energy conversion and storage devices.

Sulfidation and NaOH etching in CoFeAl LDH evolved catalysts for an efficient overall water splitting in an alkaline solution.

In this study, a hierarchical interconnected porous metal sulfide heterostructure was synthesized from CoFeAl layered double hydroxides (LDHs) by a two-step hydrothermal process (sulfidation and a NaOH etching process). Among the as-made samples, the CoFeAl-T-NaOH electrode exhibited excellent oxygen and hydrogen evolution reaction catalytic activities with overpotentials of 344 mV and 197 mV at the current density of 100 mA cm-2, respectively. Meanwhile, small Tafel slopes of 57.7 mV dec-1 and 106.5 mV dec-1 for water oxidation and hydrogen evolution were observed for the CoFeAl-T-NaOH, respectively. Serving as both the cathode and anode for overall water splitting, the CoFeAl-T-NaOH electrode reached a current density of 10 mA cm-2 at a cell voltage of 1.65 V with excellent stability. The enhanced electrocatalytic activity could be attributed to: the hierarchical interconnected nanosheet structure facilitating mass transport; the porous structure promoting electrolyte infiltration and reactant transfer; the heterojunction accelerating charge transfer; and the synergistic effect between them. This study offered a new clue for in situ synthesizing porous transition-metal based heterojunction electrocatalysts with a careful tuning of the sequence of sulfuration and alkaline etching to enhance the electrocatalytic performance.

Accelerating charge transfer for Ni(OH)2 through chlorine-anion decoration in the urea electrooxidation reaction

Chlorine-anion-modified Ni(OH)2 (Cl32–Ni(OH)2) has low crystallinity, a large specific surface area and more oxygen defects, resulting in enhanced charge transfer, ultimately facilitating the urea oxidation reaction.

Constructing SnS/Fe2O3 heterostructure anchored on few-layered graphene as an ion-adsorption/diffusion enhancer for ultrafast and cycle-stable sodium storage

Transition-metal sulfides are emerging as appealing candidates for sodium-ion batteries (SIBs) owing to their merits of high capacities and acceptable reversibilities. Fabricating heterostructure composed of two different semiconductors has been well demonstrated to effectively tackle the key issues of large volume fluctuation and poor de-/sodation kinetics. Herein, via the in-situ vulcanization of Sn with the nanospace confinement of Fe2O3 and graphene, we have constructed the micro/nanostructured SnS/Fe2O3-G heterostructure by one-step plasma-assisted milling, in which the SnS/Fe2O3 nanoclusters are tightly anchored on few-layered graphene network. Benefiting from the built-in electric field and interfacial electronic coupling between SnS and Fe2O3 nanocomponents, the SnS/Fe2O3-G heterostructure is endowed with accelerated charge transfer, enhanced Na+ diffusion/adsorption kinetics, and stable electrochemical framework, greatly improving the rate capability and cyclic stability of SnS. As expected, the SnS/Fe2O3-G heterostructure anode provides high-rate capability with high capacities of 454.3/399.2 mAh/g at 5/10 A g−1, and long-term cyclic stability with high retained capacities of 442.2/386.5 mAh/g at 1/2 A g−1 for 2000 cycles. Moreover, the assembled full battery also delivers high rate (capacity ratios of 67.1 %/54.2 % at 2/5 A g−1 relative to 0.2 A g−1) and long life (high capacity retention of 94.5 % after 200 cycles at 1 A g−1). The simple strategy and fabrication method, together with the superb performance, demonstrate that the SnS/Fe2O3-G heterostructure can be a promising anode for SIBs application.

Precisely introducing active sites into NU-1000 through linker incorporation for degrading sulfamethoxazole under visible-light photo-Fenton process

Combining adsorption and catalytic degradation to remove micropollutants in water has become a scientific challenge. However, the current material possessing both suitable pore size and evenly distributed active sites together is less common. Herein, we synthesized stable mesoporous metal–organic framework (MOFs) with Zr6 clusters and carboxylate linkers using solvent-assisted linker incorporation and post-synthetic metalation (NU-1000-Fe). A terpyridine-iron (II/III)-based metal–ligand was introduced into the porous channels successfully in Zr-MOFs without changing the mesoporous skeleton. The remained mesoporosity of the framework facilitated the adsorption of sulfamethylthiazole (SMX) in water (adsorption efficiency ∼ 40 %). Besides, it is verified that efficient p-n heterojunctions were successfully constructed by terpyridine-iron (II/III) and NU-1000. Results show that the accelerated charge transfer and photo-generated electron-hole separation abilities through introducing terpyridine-iron (II/III) facilitate the elimination of SMX in the process of visible-light photo-Fenton (removal efficiency > 90 %). Our findings offer a facile solvent-assisted ligand incorporation strategy for introducing additional active sites into MOFs to promote the degradation of micropollutants in water.

TiO2-based cathode with modest oxygen vacancies and defective Ti3+ for long-life lithium-oxygen batteries

Rational designed cathode including the surface engineering of catalyst e.g. defect creation and the precise selection of catalyst that could avoid the side reaction of carbon have been verified of great concern in achieving long-life lithium-oxygen batteries. Herein, oxygen vacancies and Ti3+ were both introduced into a tubular brush-like cathode structure, in which nano-needled TiO2 grew in situ on carbon textile (CT), and further enhancement of the catalytic performance was achieved by loading RuO2. The introduction of oxygen vacancies and Ti3+ in TiO2 could regulate the charge overpotential, and the synergistic effect between ruthenium dioxide and titanium dioxide accelerated charge transfer, and adjusted the electronic structure to achieve the surface-mediated formation mechanism of thin film lithium peroxide. Besides, TiO2 grew evenly on the surface of carbon matrix, thus restraining the carbon corrosion. Thus, CT@TiO2 and CT@TiO2-RuO2 provided low overpotentials of 0.94 V and 0.69 V and superior cycle life. Meanwhile, an ultra-long life of 317 cycles was achieved in the battery with the CT@TiO2-RuO2 cathode at a high current density of 0.3 mA cm−2.

Interface engineering of Fe3Se4/FeSe heterostructures encapsulated in MXene for boosting LiPS conversion and inhibiting shuttle effect

Developing advanced catalysts with high chemisorption toward promoting the conversion of lithium polysulfide (LiPS) is the key to the commercial application of Lithium-sulfur (Li-S) batteries. Here, a novel catalyst consisting of Fe3Se4/FeSe heterojunctions encapsulated in two-dimensional (2D) MXene nanosheets is prepared by in situ growth and selenization of Fe-MOFs. The MXene skeleton captures polysulfides effectively and the Fe3Se4/FeSe heterojunction plays a catalytic role as well as their strong synergistic effect achieves “capture-adsorption-catalysis” of LiPS. A Li-S battery with Fe3Se4/FeSe@MXene-PP separator delivers a high specific capacity (1104.2 mAh/g at 0.2C) and outstanding rate capacity (758.8 mA h g−1 at 4C). Even with sulfur loading as high as 5.8 mg cm−2, the Li-S battery has a high specific capacity of 862.6 mAh/g at 0.2C and cycle stability (92.3 % retention after 120 cycles). The involved mechanisms of performance improvement were discussed and demonstrated by density function theory (DFT) calculations and in situ Raman analysis. Interface engineering of the Fe3Se4/FeSe increases the density of states at the Fermi level, reduces the activation energy of Li2S decomposition, and the establishment of an internal electric field accelerates charge transfer. This work provides an effective approach to the design of high-performance catalysts for improved Li-S batteries.

Site-selective photocoupled electrocatalytic CO2 reduction over efficient Al-oxo chain based-porphyrin framework

Photo-coupled electrocatalytic CO2 reduction is an emerging method to promote energy efficiency of electrocatalytic CO2 reduction. However, precisely designing a precatalysts with site-selectivity for efficient photo-coupled electrocatalytic CO2 reduction is still a challenge. Here, a photo-coupled electrocatalyst bearing aluminum (Al)-oxo chain as metal node and transition metal sites as metal center, is dedicated to reducing CO2 for the first time. A satisfactory CO2-to-CO conversion is achieved for Al-PMOF(Co), showing a Faradaic efficiency as high as ∼90% and a long-term stability over 35 h under visible light. The improved performance stem from Al-oxo chain imparting high stability, atomic Co site expediting charge transfer rate (Kct) and visible light accelerating charge transfer across interface. Theoretical calculations and in situ reflection infrared spectroscopy show that the 3dz2 orbital of atomic Co site exists a large resonance with the 2p orbital of *COOH intermediate, thus inducing CO2 reduction though a favorable pathway.

Interface engineering of Mo-doped Ni9S8/Ni3S2 multiphase heterostructure nanoflowers by one step synthesis for efficient overall water splitting

Accelerating charge transfer efficiency by constructing heterogeneous interfaces on metal-based substrates is an effective way to improve the electrocatalytic performance of materials. However, minimizing the substrate-catalyst interfacial resistance to maximize catalytic activity remains a challenge. This study reports a simple interface engineering strategy for constructing Mo-Ni9S8/Ni3S2 heterostructured nanoflowers. Experimental and theoretical investigations reveal that the primary role assumed by Ni3S2 in Mo-Ni9S8/Ni3S2 heterostructure is to replace nickel foam (NF) substrate for electron conduction, and Ni3S2 has a lower potential energy barrier (0.76 to 1.11 eV) than NF (1.87 eV), resulting in a more effortless electron transfer. The interface between Ni3S2 and Mo-Ni9S8 effectively regulates electron redistribution, and when the electrons from Ni3S2 are transferred to Mo-Ni9S8, the potential energy barriers at the heterogeneous interface are 1.06 eV, lower than that between NF and Ni3S2 (1.53 eV). Mo-Ni9S8/Ni3S2-0.1 exhibited excellent oxygen evolution reaction (OER)/hydrogen evolution reaction (HER) bifunctional catalytic activity in 1 M KOH, with overpotentials of only 223 mV@100 mA cm−2 for OER and 116 mV@10 mA cm−2 for HER. Moreover, when combined with an alkaline electrolytic cell, it required only an ultra-low cell voltage of 1.51 V to drive a current density of 10 mA cm−2. This work provides new inspirations for rationally designing interface engineering for advanced catalytic materials.

Boosting the Electrochemical Detection Response Toward Hydroxychloroquine via Tungsten Trioxide Nanorods/Nitrogen-Doped Carbon Nanofiber Nanocomposite

The overusage of hydroxychloroquine (HQ) amidst the outbreak of coronavirus disease has contributed to increased fatalities concerning HQ poisoning. Hence, there is an utmost requirement to develop accurate and onsite methodologies for monitoring HQ in biological samples and water bodies. Metal-oxide-decorated carbon nanomaterials present excellent electrocatalytic properties, contributing to improved sensor responses. This study introduces tungsten trioxide nanorods/nitrogen-doped carbon nanofiber (WO3/N-CNF) nanocomposite, capable of detecting HQ electrochemically. The conjunction of WO3 with N-CNF offers accelerated charge transfer kinetics with an abundance of surface-active sites that benefit the sensing mechanism. Furthermore, synergistic effects arising from the nanocomposite augment the conductivity and promote faster ion diffusion. The WO3/N-CNF-based electrochemical sensor deliver high performance in the working concentration range of 0.007–480 μM and provides a detection limit of 2.0 nM for HQ. The fabricated sensor has excellent operational stability and reproducibility and is also able to show a superb selectivity toward HQ in comparison to various interfering compounds. This indicates that the designed WO3/N-CNF nanocomposite can be used as a potential electrocatalyst for the real-time monitoring of HQ.

Boosting Electrocatalytic Ammonia Synthesis of Bio-Inspired Porous Mo-Doped Hematite via Nitrogen Activation.

Electrochemical N2 reduction reaction (NRR) emerges as a highly attractive alternative to the Haber-Bosch process for producing ammonia (NH3) under ambient circumstances. Currently, this technology still faces tremendous challenges due to the low ammonia production rate and low Faradaic efficiency, urgently prompting researchers to explore highly efficient electrocatalysts. Inspired by the Fe-Mo cofactor in nitrogenase, we report Mo-doped hematite (Fe2O3) porous nanospheres containing Fe-O-Mo subunits for enhanced activity and selectivity in the electrochemical reduction from N2 to NH3. Mo-doping induces the morphology change from a solid sphere to a porous sphere and enriches lattice defects, creating more active sites. It also regulates the electronic structures of Fe2O3 to accelerate charge transfer and enhance the intrinsic activity. As a consequence, Mo-doped Fe2O3 achieves effective N2 fixation with a high ammonia production rate of 21.3 ± 1.1 μg h-1 mgcat.-1 as well as a prominent Faradaic efficiency (FE) of 11.2 ± 0.6%, superior to the undoped Fe2O3 and other iron oxide catalysts. Density functional theory (DFT) calculations further unravel that the Mo-doping in Fe2O3 (110) narrows the band gap, promotes the N2 activation on the Mo site with an elongated N≡N bond length of 1.132 Å in the end-on configuration, and optimizes an associative distal pathway with a decreased energy barrier. Our results may pave the way toward enhancing the electrocatalytic NRR performance of iron-based materials by atomic-scale heteroatom doping.

Magnetoelectric Coupling for Metal–Air Batteries

AbstractMetal–air batteries have become one of the new potential sources of electrochemical energy due to the excellent electrochemical characteristics, environmental friendliness and cheap cost. Whereas, the commercialization of the metal–air batteries is still subject to the sluggish kinetics on air electrode and hydrogen evolution corrosion as well as dendrite growth of metal anode. Recently, the applied magnetic field, as a technology for transferring energy across physical space, receives more attention, can improve the performance of metal–air batteries by promoting mass transfer, accelerating charge transfer and enhancing electrocatalytic ability based on magnetohydrodynamic effect, Kelvin force effect, Hall effect, Spin selectivity effect, Maxwell stress effect and Magnetothermal effect. This review provides the recent progress in the research on the relative mechanism and characteristic of the magnetic field in the metal–air batteries.

CoNi bimetallic alloy cocatalyst-modified TiO2 nanoflowers with enhanced photocatalytic hydrogen evolution

In terms of improving photocatalytic hydrogen production performance, inexpensive and earth-rich cocatalysts have become promising alternatives to precious metals. Herein, a novel CoNi–TiO2 photocatalyst composed of TiO2 nanoflowers and CoNi alloy was prepared by hydrothermal and chemical reduction methods. Various characterizations and test results have confirmed that the further improvement of the photocatalytic performance of the CoNi–TiO2 photocatalyst is mainly due to the fact that the bimetallic CoNi alloy can accelerate charge transfer and inhibit the recombination of photo-induced carriers. The hydrogen production rate of the prepared CoNi–TiO2 is about 24 times higher than that of the pristine TiO2, and its hydrogen production rate value can reach 6580.9 μmol g−1 h−1, and showing comparable photocatalytic performance to 0.5 wt% Pt–TiO2. In addition, combined with the characterization results, a probable mechanism for enhanced photocatalytic performance was proposed. This study provides favorable enlightenment for the design of a series of highly efficient non-precious metal TiO2-based photocatalysts.

Uneven crystallization of lead halide perovskite in the carbon-electrode based, low-temperature mesoscopic perovskite solar cells

Crystallization of perovskite is monitored in carbon-electrode based, low-temperature, mesoscopic perovskite solar cells. Crystallographic and morphological properties of the perovskite are examined through changes in the film thickness of carbon-electrode or the volume of perovskite precursor. It is observed that, when a relatively thin carbon-electrode or large volume of perovskite precursor is used, perovskite crystallites mainly form on the device surface, leaving the bottom part of the device un-wetted. However, if a thicker carbon-electrode or less perovskite precursor is used, crystallization could be seen in the whole porous skeleton, and relative uniform distribution of perovskite crystallites is achieved. As such, uneven crystallization is observed. Such behavior is due to solvent evaporation on the surface, which facilitates nucleation processes on the surface, while retards crystallization on the bottom due to the Ostwald ripening effect. Charge transfer/recombination processes and photo-to-electric power conversion properties are studied. As expected, uneven crystallization results in retarded charge transfer and increased risk of recombination, and poor power conversion efficiency, for example, ∼3%. In contrast, uniform crystallization accelerates charge transfer and reduces recombination risk, and increases the efficiency to higher than 11% (AM1.5G, 100 mW/cm2).

Construction of Fe(III) doping modified AgI/NH2-MIL-68(In/Fe) Z-scheme heterojunction photocatalysts through unique internal and interfacial charge transmission and separation efficiency

The development of highly efficient strategy to facilitate comprehensive charge transmission and effective spatial charge separation is expected as a promising approach to improve photocatalytic performance. Herein, the Fe(III) doping modified AgI/NH2-MIL-68(In/Fe) Z-scheme heterojunction (ANM-x composite) with unique internal and interfacial charge transmission performance was fabricated by a facile ion exchange precipitation method. The optimized ANM-50 composite exhibits the maximum photocatalytic activity for the degradation of tetracycline, which is about 9.54, 2.61 and 1.86 times higher than that of pure NH2-MIL-68In, NH2-MIL-68(In/Fe) and AgI, respectively. The characterization results displayed that Ag nanoparticles (NPs) were generated during the photocatalytic procedure, which not only served as a charge transfer-highway, but also reduced the charge flow energy barrier, thereby accelerating charge transfer efficiency and consolidating the stability of the Z-scheme heterojunction. Mechanism exploration reflected that the superior photocatalytic performance was associated with synergetic effect among the introduced Fe(III), constructed ANM Z-scheme heterojunction and the generated Ag NPs, which significantly expands visible light response range and promotes more effective internal and interfacial charge separation. This research not only designs an efficient photocatalyst for decomposing tetracycline, but also opens a new perspective for rational developing Z-scheme heterojunction with unique internal and interfacial charge flow steering.

Achieving highly efficient pH-universal hydrogen evolution by Mott-Schottky heterojunction of Co2P/Co4N

A vital step towards sustainable hydrogen production is to develop high-efficiency electrocatalysts for pH-universal hydrogen evolution reaction (HER). Modulation of the electronic structure of electrocatalysts by constructing Mott-Schottky heterojunction could be regarded as an effective strategy to promote the electrochemical performances. Herein, we report hybrid Mott-Schottky electrocatalyst composed of metallic Co4N and n-type semiconducting Co2P,fabricated via the hydrothermal method followed by the subsequent phosphating and nitriding treatment. Due to the Mott-Schottky effect, the self-driven charge carriers transfer occurs at the heterointerfaces of Co2P/Co4N, leading to a built-in electric field, accelerated charge transfer rate, and improved chemisorption free energies of the reaction intermediates, ultimately boosting the dissociation of water molecules. Therefore, the as-prepared Co2P/Co4N electrocatalyst exhibits outstanding pH-universal HER performance with extremely low overpotentials of 53, 19, and 32 mV at a current density of 10 mA cm−2 in 0.5 M H2SO4, 1 M phosphate buffer solution (PBS), and 1 M KOH electrolytes, respectively. Further, the electrocatalyst reveals low Tafel slopes of 38, 26, and 50 mV dec−1, which outperform those of the previously reported Co-based catalysts. Density functional theory (DFT) calculations clarify that the Schottky contact can regulate the adsorption energy of water, and the electronic structure at interface of the heterojunction weakens the hydrogen adsorption free energy (ΔGH*) of Co2P/Co4N to nearly zero, which is the reason for the addressed splendid HER performance.

N-doped carbon layer promoted charge separation/transfer in WP/g-C3N4 heterostructures for efficient H2 evolution and 4-nitrophenol removal

Monodispersed WP nanoparticles were encapsulated in nitrogen-doped carbon (NC) layers via thermal polymerization at high temperature. The intimate interface between WP and NC accelerated charge transfer and elevated the electroconductivity. As-prepared WP@NC nanocomposites revealed enhanced electrocatalytic hydrogen evolution reaction (HER) activities in both of acidic and alkaline electrolytes with Tafel slopes of 73 and 85 mv/dec, respectively. Furthermore, WP@NC nanocomposites instead of noble metal co-catalysts were loaded on superior thin g-C3N4 nanosheets (CN) by thermal polymerization at different temperature. In the case of without Pt, the photocatalytic hydrogen generation rate of CN/WP@NC heterojunctions prepared using optimized conditions reached 1217.6 μmol g−1 h−1, which was ∼196 folds of pure g-C3N4 nanosheets. This is ascribed to that N-doped carbon layers on WP improved the separation and transfer efficiency of photogenerated charge carriers. Interestingly, the carbon layers improved the chemical stability and corrosion resistance to ensure enhanced photocatalytic hydrogen generation in simulated seawater. In addition, the sample revealed outstanding light-assisted elimination capability of 4-nitrophenol (4-NP) because of the selective hydrogenation reaction to 4-aminophenol and photodegradation reaction of 4-NP. Under visible light irradiation, the removal efficiency using CN/WP@NC reached 99% within 10 min. The kinetic constant (0.443 min−1) was 17.8 times of that of g-C3N4 nanosheets. This work supplied an efficient method to fabricate bi-functional noble-metal-free catalyst towards clean energy production and environment remediation.

Boosted solar water photoreduction by conjugated polymer-mediated tandem charge transfer

Semiconductor materials anchored with transition metal cluster are promising photocatalysts for photocatalytic hydrogen evolution. In this paper, Co, N-co-doped graphene modified thin mesoporous carbon nitride (Co-NG/TMCN) was be synthesized through electrostatic adsorption treatment. Extensive characterization was used to explore the morphology, structures and optical properties of the as-prepared photocatalysts. The 10 wt% Co-NG/TMCN exhibited the high photocatalytic hydrogen evolution rate (2949 μmol g−1) within 4 h visible light irradiation, which was about 113 times than that of the pure TMCN (26 μmol g−1). Co-NG material with excellent electrical conductivity played a major role in accelerating charge transfer from TMCN material to cobalt atomic clusters. The photocatalytic hydrogen evolution performance of Co-NG/TMCN material was effectively improved. Consequently, a feasible approach for doping transition metal clusters to enhance photocatalytic activity was provided.