Charge Transfer Channel Research Articles

Self-assembly of N,S-MXene/3DPC heterostructure with multiple charge transfer channels for high-performance supercapacitors and sodium-ion batteries

Individual MXene (Ti3C3Tx) films tend to re-accumulate, seriously reducing the electrochemical properties. Herein, a viable hydrothermal method is being adopted to achieve the self-assembly of N and S co-doped three-dimensional porous carbon (3DPC) with conductive networks and MXene. For SCs, the N,S-MXene/3DPC electrode displays 412.7 F g−1 at 1 A g−1. When all-solid-state asymmetric SCs (ASCs) are manufactured with active carbon, the N,S-MXene/3DPC//AC ASCs present 210.5 F g−1 at 1 A g−1 and retain 97.5% of initial cycle through 5000 rotations. The energy density reaches its maximum of 94.7 Wh kg−1 at 900 W kg−1. In addition, the N,S-MXene/3DPC anode of SIBs demonstrates a reversible capability of 465.5 mAh g−1 at 0.2 A g−1. It also sustains a remarkable 72.9% preservation of capacity over 1000 rotations at 2.0 A g−1. The excellent electrochemical performance is attributed to following points: 3DPC with conductive networks can provide multiple transfer paths for ions and charges and support MXene. The co-doping of N and S for 3DPC can provide numerous active sites for electrochemical reactions, while the addition of MXene improves conductivity and mechanical stability. The N,S-MXene/3DPC material and its preparation method exhibit great potential for application in the field of electrochemical energy storage.

Interfacial Si–O–Zr bonds induced well dispersed zirconia on magnetic mesoporous silicas for enhanced tetracycline removal

Constructing recoverable materials with both high adsorption capacity and excellent photocatalytic performance towards antibiotics elimination is very meaningful and challenging in wastewater remediation. In this work, we demonstrate a simple interface engineering strategy to design well dispersed zirconia on core–shell structured magnetic mesoporous silica microspheres (MMS) for efficient removal of tetracycline hydrochloride (TC). With ultrahigh specific surface area (682.0 m2/g) and interfacial Si-O-Zr serving as active sites, the optimal sample (MMS-Zr10) exhibits enhanced TC adsorption capacity of 266.5 mg/ZrO2 g, which is 19.2-fold than that of pure ZrO2. Simultaneously, the photocatalytic degradation rate constant of TC over MMS-Zr10 in the presence of peroxydisulfate (PDS) is 12.5 times that of ZrO2 under visible light irradiation, which may be attributed to the enhanced light harvest capability and high charge separation efficiency facilitated by interfacial Zr–O–Si charge transfer channels. Furthermore, in consecutive adsorption cycles in both deionized (DI) water solution and actual wastewater, no obvious decline in TC removal % is observed. The TC adsorption is mainly governed by pore filling, hydrogen bonding and electrostatic interactions; whilst O2•−, h+, SO4•−, •OH and 1O2 species are responsible for enhanced photocatalytic degradation of TC.

Building a Charge Transfer Bridge between g-C3N4 and Perovskite with Molecular Engineering to Achieve Efficient Perovskite Solar Cells.

Effective defect passivation and efficient charge transfer within polycrystalline perovskite grains and corresponding boundaries are necessary to achieve highly efficient perovskite solar cells (PSCs). Herein, focusing on the boundary location of g-C3N4 during the crystallization modulation on perovskite, molecular engineering of 4-carboxyl-3-fluorophenylboronic acid (BF) on g-C3N4 was designed to obtain a novel additive named BFCN. With the help of the strong bonding ability of BF with both g-C3N4 and perovskite and favorable intramolecular charge transfer within BFCN, not only has the crystal quality of perovskite films been improved due to the effective defects passivation, but the charge transfer has also been greatly accelerated due to the formation of additional charge transfer channels on the grain boundaries. As a result, the champion BFCN-based PSCs achieve the highest photoelectric conversion efficiency (PCE) of 23.71% with good stability.

High-efficiency photocatalytic CO2 reduction enabled by interfacial Ov and isolated Ti3+ of g-C3N4/TiO2 Z-scheme heterojunction

Exploring the real force that drives the separation of Coulomb-bound electron-hole pairs in the interface of heterojunction photocatalysts can establish a clear mechanism for efficient solar energy conversion efficiency. Herein, the formation of oxygen vacancy (Ov) and isolated Ti3+ was precisely regulated at the interface of g-C3N4/TiO2 Z-scheme heterojunction (g-C3N4/Ov-Ti3+-TiO2) by optimizing the opening degree of the calcination system, showing excellent production rate of CO and CH4 from CO2 photoreduction under visible light. This photocatalytic system also exhibited prominent stability. Combining theoretical calculation and characterization, the introduction of Ov and isolated Ti3+ on the interface could construct a charge transfer channel to break the forbidden transition of n → π*, improving the separation process of photoexcited electron-hole pairs. The photoexcited electrons weakened the covalent interaction of CO bonds to promote the activation of adsorbed inert CO2 molecules, significantly reducing the energy barrier of the rate-limiting step during CO2 reduction. This work demonstrates the great application potential of reasonably regulating heterojunction interface for efficient photocatalytic CO2 reduction.

Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Z-scheme heterojunctions with enhanced photocatalytic hydrogen production

Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Z-scheme heterojunctions with enhanced photocatalytic hydrogen production

Innovative Catalyst Design of Sea-Urchin-like NiCoP Nanoneedle Arrays Supported on N-Doped Carbon Nanospheres for Enhanced HER Performance.

Hydrogen (H2) stands as a clean energy alternative to fossil fuels, especially within the domain of the hydrogen evolution reaction (HER), offering prospective solutions to mitigate both environmental and energy-related challenges. In this work, we successfully synthesized a sea-urchin-like catalyst, specifically a nickel-cobalt phosphide nanoneedle array on N-doped carbon nanospheres (Ni0.5Co1.5P@NCSs), for efficient HER by a sequential hydrothermal and low-temperature phosphating process. The catalyst exhibits sea-urchin-like structures, offering a specific surface area of 298 m2 g-1 and consequently furnishing a greater abundance of active sites. Comparing with non-sea-urchin-like Ni0.5Co1.5P@CN catalysts, the Ni0.5Co1.5P@NCSs exhibit an overpotential of 163 mV at 10 mA cm-2, a Tafel slope of 60 mV dec-1, and a maintained current density of approximately 90% during 50 h of continuous electrolysis. Experiments demonstrate that the outstanding electrochemical properties of the Ni0.5Co1.5P@NCSs originate from nitrogen doping of carbon spheres, the distinctive morphology of sea-urchin-like nanoneedle arrays, and simultaneous enhancements in intermediate adsorption energy, charge transfer, and electrolyte diffusion channel shortening. This work emphasizes a preparation strategy for synthesizing an attractive electrocatalyst with a low cost and efficient HER performance.

Insights into interfacial S-scheme/bulk type II dual charge transfer mechanism enabling silver oxide/N-rich carbon nitride anti-photocorrosion and enhanced photoactivity

Infectious diseases, such as COVID-19, continue to pose a significant threat to global public health and economics. This study establishes a one-of-a-kind heterojunction catalyst with a built-in electric field and enhanced structural defects, allowing for the formation of interfacial S-scheme and bulk type-II dual charge transfer channels, as demonstrated by extensive experimental investigation and density functional theory calculations. This unique property greatly enhances the photogenerated electron/hole pair separation and transfer, producing more active species in Ag2O/C3N5 for water disinfection, which inactivation efficiency of E. coli is around 7.0 folds for pure C3N5 and 1.5 folds for Ag2O. The spatial separation of photogenerated e-/h+ pairs and the tendency of O2/H2O molecules to be reduced or oxidized at the interface enable excellent anti-photocorrosion. Exceptional disinfection of real lake and river water, along with exceptional stability and reusability, demonstrate the practical application potential. This work is pivotal for the theoretical development of sophisticated photocatalytic systems.

Triphasic Ni2P-Ni12P5-Ru with Amorphous Interface Engineering Promoted by Co Nano-Surface for Efficient Water Splitting.

This research designs a triphasic Ni2P-Ni12P5-Ru heterostructure with amorphous interface engineering strongly coupled by a cobalt nano-surface (Co@NimPn-Ru) to form a hierarchical 3D interconnected architecture. The Co@NimPn-Ru material promotes unique reactivities toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline media. The material delivers an overpotential of 30mV for HER at 10mAcm-2 and 320mV for OER at 50 mAcm-2 in freshwater. The electrolyzer cell derived from Co@NimPn-Ru(+,-) requires a small cell voltage of only 1.43V in alkaline freshwater or 1.44V in natural seawater to produce 10mA cm-2 at a working temperature of 80°C, along with high performance retention after 76h. The solar energy-powered electrolyzer system also shows a prospective solar-to-hydrogen conversion efficiency and sufficient durability, confirming its good potential for economic and sustainable hydrogen production. The results are ascribed to the synergistic effects by an exclusive combination of multi-phasic crystalline Ni2P, Ni12P5, and Ru clusters in presence of amorphous phosphate interface attached onto cobalt nano-surface, thereby producing rich exposed active sites with optimized free energy and multi open channels for rapid charge transfer and ion diffusion to promote the reaction kinetics.

P-N Bonds-Mediated Atomic-Level Charge-Transfer Channel Fabricated between Violet Phosphorus and Carbon Nitride Favors Charge Separation and Water Splitting.

Heterostructures are widely employed in photocatalysis to promote charge separation and photocatalytic activity. However, their benefits are limited by the linkages and contact environment at the interface. Herein, violet phosphorus quantum dots (VPQDs) and graphitic carbon nitride (g-C3N4) are employed as model materials to form VPQDs/g-C3N4 heterostructures by a simple ultrasonic pulse excitation method. The heterostructure contains strong interfacial P-N bonds that mitigate interfacial charge-separation issues. P-P bond breakage occurs in the distinctive cage-like [P9] VPQD units during longitudinal disruption, thereby exposing numerous active P sites that bond with N atoms in g-C3N4 under ultrasonic pulse excitation. The atomic-level interfacial P-N bonds of the Z-scheme VPQDs/g-C3N4 heterostructure serve as photogenerated charge-transfer channels for improved electron-hole separation efficiency. This results in excellent photocatalytic performance with a hydrogen evolution rate of 7.70mmolg-1h-1 (over 9.2 and 8.5 times greater than those of pure g-C3N4 and VPQDs, respectively) and apparent quantum yield of 11.68% at 400nm. Using atomic-level chemical bonds to promote interfacial charge separation in phosphorene heterostructures is a feasible and effective design strategy for photocatalytic water-splitting materials.

Creation of Interfacial S4-Sn-N2 Electron Pathways for Efficient Light-Driven Hydrogen Evolution.

Establishing effective charge transfer channels between two semiconductors is key to improving photocatalytic activity. However, controlling hetero-structures in situ and designing binding modes pose significant challenges. Herein, hydrolytic SnCl2·2H2O is selected as the metal source and loaded in situ onto a layered carbon nitriden supramolecular precursor. A composite photocatalyst, S4-Sn-N2, with electron pathways of SnS2 and tubular carbon nitriden (TCN) is prepared through pyrolysis and vulcanization processes. The contact interface of SnS2-TCN is increased significantly, promoting the formation of S4-Sn-N2 micro-structure in a Z-scheme charge transfer channel. This structure accelerates the separation and transport of photogenerated carriers, maintains the stronger redox ability, and improves the stability of SnS2 in this series of heterojunctions. Therefore, the catalyst demonstrated exceptional photocatalytic hydrogen production efficiency, achieving a reaction rate of 86.4µmolh-1, which is 3.15 times greater than that of bare TCN.

Novel Ag-Bridged Z-Scheme CdS/Ag/Bi2WO6 Heterojunction: Excellent Photocatalytic Performance and Insight into the Underlying Mechanism

The construction of semiconductor heterojunction photocatalysts that improve the separation and transfer of photoinduced charge carriers is an effective and widely employed strategy to boost photocatalytic performance. Herein, we have successfully constructed a CdS/Ag/Bi2WO6 Z-scheme heterojunction with an Ag-bridge as an effective charge transfer channel by a facile process. The heterostructure consists of both CdS and Ag nanoparticles anchored on the surface of Bi2WO6 nanosheets. The photocatalytic efficiency of the CdS/Ag/Bi2WO6 system was studied by the decontamination of tetracycline (TC) and Rhodamine B (RhB) under visible light irradiation (λ ≥ 420). The results exhibited that CdS/Ag/Bi2WO6 shows markedly higher photocatalytic performance than that of CdS, Bi2WO6, Ag/Bi2WO6, and CdS/Bi2WO6. The trapping experiment results verified that the •O2− and h+ radicals are the key active species. The results of photoluminescence spectral analysis and photocurrent responses indicated that the CdS/Ag/Bi2WO6 heterojunctions exhibit exceptional efficiency in separating and transferring photoinduced electron−hole pairs. Based on a series of characterization results, the boosted photocatalytic activity of the CdS/Ag/Bi2WO6 system is mostly due to the successful formation of the Ag-bridged Z-scheme heterojunction; these can not only inhibit the recombination rate of photoinduced charge carriers but also possess a splendid redox capacity. The work provides a way for designing a Z-scheme photocatalytic system based on Ag-bridged for boosting photocatalytic performance.

Enhanced Photocatalytic Properties of All-Organic IDT-COOH/O-CN S-Scheme Heterojunctions Through π-π Interaction and Internal Electric Field.

Herein, we present a distinct methodology for the in situ electrostatic assembly method for synthesizing a conjugated (IDT-COOH)/oxygen-doped g-C3N4 (O-CN) S-scheme heterojunction. The electron delocalization effect due to π-π interactions between O-CN and self-assembled IDT-COOH favors interfacial charge separation. The self-assembled IDT-COOH/O-CN exhibits a broadened visible absorption to generate more charge carriers. The internal electric field between the IDT-COOH and the O-CN interface provides a directional charge-transfer channel to increase the utilization of photoinduced charge carriers. Moreover, the active species (•O2-, h+, and 1O2) produced by IDT-COOH/O-CN under visible light play important roles in photocatalytic disinfection. The optimum 40% IDT-COOH/O-CN can kill 7-log of methicillin-resistant Staphylococcus aureus (MRSA) cells in 2 h and remove 88% tetracycline (TC) in 5 h, while O-CN only inactivates 1-log of MRSA cells and degrades 40% TC. This work contributes to a promising method to fabricate all-organic g-C3N4-based S-scheme heterojunction photocatalysts with a wide range of optical responses and enhanced exciton dissociation.

Modification of a rod-shaped Bi-MOF with MoS2 nanosheets to form a p-n heterojunction for enhanced antimicrobial activity

A novel visible-light-driven type II p-n heterojunction CAU-17/MoS2 photocatalytic antifouling biocide was prepared and indicated significant inhibition against the most pharmaceutically recognized harmful microorganisms: gram-positive Staphylococcus aureus (S. aureus), gram-negative Escherichia coli (E. coli) and the drug-resistant bacterium methicillin-resistant Staphylococcus aureus (MRSA). The antimicrobial mechanism is attributed to the production of reactive oxygen species (ROS) such as •OH, 1O2 due to the photocatalytic properties of CAU-17/MoS2 heterojunction. The electron-hole complexation efficiency of the nanocomposites was analyzed using photoluminescence spectroscopy and characterized using electron microscope. It was found that the heterojunction structure of the nanocomposites provided multiple charge transfer channels to significantly improve the transporting and separating efficiency for the photo-induced electron-hole pairs, which consequently facilitated the production of ROS. Given the promising antimicrobial effects, further investigation on the broader application of CAU-17/MoS2 biocides is needed to test the cytotoxicity, as well as the post-bacteriostatic wound healing effect upon animal models.

Visible-light-driven tetracycline hydrochloride degradation via ZnTi-LDHs/Ce2S3 Z-scheme heterojunctions: Performance and mechanistic analysis

The refractory and hard-to-dispose tetracycline hydrochloride (TC) poses an enormous threat to human health and the water environment. Herein, a novel Z-scheme ZnTi-LDHs/Ce2S3 heterojunction photocatalyst was successfully developed for TC degradation under visible light conditions. This sophisticated material demonstrated a remarkable degradation rate of 0.0124 min−1, marking a noteworthy advancement compared to ZnTi-LDHs, Ce2S3, and the commonly reported LDHs/LDHs-based composites, with an approximate one-order-of-magnitude improvement. The inherent synergy between Ce2S3 and LDHs manifested as a Z-scheme charge transfer channel, augmenting visible-light absorption, and fostering carrier separation. Both O2·- and h+ played critical roles in the TC degradation process, mediating reductive and oxidative pathways, respectively. ZnTi-LDHs/Ce2S3 demonstrated robust reusability and broad applicability for degrading diverse dyes and antibiotics. This work demonstrated a promising protocol for crafting efficient Z-scheme heterojunction photocatalysts based on LDHs and expanded our understanding and potential applications of photocatalytic degradation mechanisms for antibiotics.

Highly Crystalline Poly(heptazine imide)-Based Carbonaceous Anodes for Ultralong Lifespan and Low-Temperature Sodium-Ion Batteries.

Carbon nitrides with layered structures and scalable syntheses have emerged as potential anode choices for the commercialization of sodium-ion batteries. However, the low crystallinity of materials synthesized through traditional thermal condensation leads to insufficient conductivity and poor cycling stability, which significantly hamper their practical applications. Herein, a facile salt-covering method was proposed for the synthesis of highly ordered crystalline C3N4-based all-carbon nanocomposites. The sealing environment created by this strategy leads to the formation of poly(heptazine imide) (PHI), the crystalline phase of C3N4, with extended π-conjugation and a fully condensed nanosheet structure. Meanwhile, theoretical calculations reveal the high crystallinity of C3N4 significantly reduces the energy barrier for electron transition and enables the generation of efficient charge transfer channels at the heterogeneous interface between carbon and C3N4. Accordingly, such nanocomposites present ultrastable cycling performances over 5000 cycles, with a high reversible capacity of 245.1 mAh g-1 at 2 A g-1 delivered. More importantly, they also exhibit an outstanding low-temperature capacity of 196.6 mAh g-1 at -20 °C. This work offers opportunities for the energy storage use of C3N4 and provides some clues for developing long-life and high-capacity anodes operated under extreme conditions.

Secondary donor-acceptor group enable efficient pure green organic light-emitting devices based on multi-resonance TADF emitters

Multi-resonance thermally activated delayed fluorescence (MR-TADF) presents great potential for applications in high-quality organic light emitting diodes (OLEDs) displays due to their superb properties of high color purity and high quantum efficiencies. Nonetheless, most reported MR-TADF emitters show unsatisfactory devices performances with severe efficiency roll-off resulted from their inherent issues of slow reverse intersystem crossing rate (kRISC) and aggregation-caused quenching (ACQ). Herein, we propose a novel strategy by employing quinazoline derivatives as secondary acceptor (PQ) and secondary donor–acceptor (PQCz) to provide intermediate locally excited triplet (3LE) states and then enhance spin-orbital coupling (SOC). In addition, the secondary donor–acceptor group PQCz in tCzBN-PQCz can suppress intermolecular interaction and provide dual long-range charge transfer (LRCT) channels to further enhance kRISC. Therefore, tCzBN-PQ and tCzBN-PQCz exhibit high kRISC of 5.6 × 105 s−1 and 7.3 × 105 s−1 with large photoluminescence quantum yield (PLQY) of 89 % and 95 % respectively. Consequently, OLED based on tCzBN-PQ and tCzBN-PQCz show excellent external quantum efficiency (EQE) of 30.2 % and 35.1 % with small efficiency roll-off and small full width at half maxima (FWHM) of 37 nm and 34 nm respectively. Especially, tCzBN-PQCz exhibits better performances and less-sensitive to the doping concentration which proves the effectiveness of this secondary donor–acceptor group.

Three-Dimensional Multihierarchical Hexagonal/Cubic ZnIn2S4 S-Scheme Heterophase Junction for Superior Photocatalysis.

It is an important strategy to design composite materials with a special microstructure and a tunable electronic structure through structural compatibility. In this work, a novel hexagonal/cubic ZnIn2S4 polymorphic heterophase junction with a three-dimensional multihierarchical structure is successfully constructed by in situ growth of hexagonal ZnIn2S4 nanosheets on the surface of cubic ZnIn2S4 flower-like microspheres prepared by topological chemical synthesis. On the one hand, the multihierarchical architecture provides large specific surface area, abundant active sites, and excellent light trapping capability. On the other hand, the construction of a direct S-scheme heterophase junction enables the formation of a special charge-transfer channel under the force of a built-in electric field, which not only improves the separation efficiency of carriers but also ensures the stronger reaction activity of charges. The prepared ZnIn2S4 heterophase junction composite photocatalyst exhibits greatly boosted photocatalytic efficiency in rhodamine B degradation, hexavalent chromium reduction, and water splitting for hydrogen production, which are 12.3, 6.5, and 3.1 times higher than that of pure hexagonal ZnIn2S4 and 8.1, 5.1, and 2.3 times higher than that of pure cubic ZnIn2S4, respectively, demonstrating its significant potential for applications in energy and environmental fields.

Efficient Photosynthesis of Hydrogen Peroxide by Cyano-Containing Covalent Organic Frameworks from Water, Air and Sunlight.

The insufficient exciton (e- -h+ pair) separation/transfer and sluggish two-electron water oxidation are two main factors limiting the H2 O2 photosynthetic efficiency of covalent organic frameworks (COFs) photocatalysts. Herein, we present an alternative strategy to simultaneously facilitate exciton separation/transfer and reduce the energy barrier of two-electron water oxidation in COFs via a dicyano functionalization. The in situ characterization and theoretical calculations reveal that the dicyano functionalization improves the amount of charge transfer channels between donor and acceptor units from two in COF-0CN without cyano functionalization to three in COF-1CN with mono-cyano functionalization and four in COF-2CN with dicyano functionalization, leading to the highest separation/transfer efficiency in COF-2CN. More importantly, the dicyano group activates the neighbouring C atom to produce the key *OH intermediate for effectively reducing the energy barrier of rate-determining two-electron water oxidation in H2 O2 photosynthesis. The simultaneously enhanced exciton separation/transfer and two-electron water oxidation in COF-2CN result in high H2 O2 yield (1601 μmol g-1 h-1 ) from water and oxygen without using sacrificial reagent under visible-light irradiation. COF-2CN can effectively yield H2 O2 in water with wide pH range, in different real water samples, in scaled-up reactor under natural sunlight irradiation, and in continuous-flow reactor for consecutively producing H2 O2 solution for water decontamination.

Efficient Photosynthesis of Hydrogen Peroxide by Cyano‐Containing Covalent Organic Frameworks from Water, Air and Sunlight

AbstractThe insufficient exciton (e−‐h+ pair) separation/transfer and sluggish two‐electron water oxidation are two main factors limiting the H2O2 photosynthetic efficiency of covalent organic frameworks (COFs) photocatalysts. Herein, we present an alternative strategy to simultaneously facilitate exciton separation/transfer and reduce the energy barrier of two‐electron water oxidation in COFs via a dicyano functionalization. The in situ characterization and theoretical calculations reveal that the dicyano functionalization improves the amount of charge transfer channels between donor and acceptor units from two in COF‐0CN without cyano functionalization to three in COF‐1CN with mono‐cyano functionalization and four in COF‐2CN with dicyano functionalization, leading to the highest separation/transfer efficiency in COF‐2CN. More importantly, the dicyano group activates the neighbouring C atom to produce the key *OH intermediate for effectively reducing the energy barrier of rate‐determining two‐electron water oxidation in H2O2 photosynthesis. The simultaneously enhanced exciton separation/transfer and two‐electron water oxidation in COF‐2CN result in high H2O2 yield (1601 μmol g−1 h−1) from water and oxygen without using sacrificial reagent under visible‐light irradiation. COF‐2CN can effectively yield H2O2 in water with wide pH range, in different real water samples, in scaled‐up reactor under natural sunlight irradiation, and in continuous‐flow reactor for consecutively producing H2O2 solution for water decontamination.

Regulating carrier transfer route via 1D-2D junction on TiO2 nanorods intercalated with N-doped γ-graphyne nanosheets

One-dimensional TiO2 nanostructure has been widely studied in the domain of photoelectrochemical water splitting. Nevertheless, the wide bandgap and fast carriers recombination of TiO2 restrain its performance. In this study, two-dimensional N-doped γ-graphyne nanosheets were synthesized and employed in the reasonable design of TiO2 heterostructure, facilitating carrier migration and water oxidation reaction. The photocurrent density of photoanode composed of N-doped γ-graphyne/TiO2 nanorods reaches 1.48 mA cm−2, 1.72 times that of pristine TiO2 at a bias of 1.23 V (vs. RHE). Meanwhile, the calculated applied bias photon-to-current efficiency increases from 0.25 % to 0.56 %. The combination of TiO2 nanorods with layered semiconductive N-doped γ-graphyne contributes to the construction of charge transfer channels, regulating surface states and reaction sites, promoting the hole storage, and reducing the free energy barrier in the velocity determination process. This study sheds light on the design of N-doped γ-graphyne modified catalysts and facilitates their application in photoelectrochemical and photoelectrocatalytic fields.