Stabilizing Unsaturated S at Interface for the Enhanced Photothermal Evolution of CH4 From CO2 DOI Open Access

An Chao,

Jun Zhang, Liang Mao

et al.

Advanced Sustainable Systems, Journal Year: 2025, Volume and Issue: unknown

Published: March 16, 2025

Abstract Highly selective photocatalytic CO 2 reduction (PCR) to methane is restricted severely due the multiple consecutive proton‐coupled electron transfer steps and stabilization of crucial intermediates. Herein, an In O 3 /CuInS composite with multifunction meticulously fabricated via heterojunction engineering achieves a remarkable selectivity CH 4 (95.73%) yield 54.9 umol·g −1 ·h . The electrons are enriched around S atoms form unsaturated sites, thereby improving efficiency reactions involving electrons. interfacial effect induces electron/photogenerated from suppressing excessive oxidation states reducing local positive charge accumulation, stabilizing sites. Unsaturated sites acts as electron‐rich centers for adsorption activation function, enhancing coverage * species on surface photocatalyst lowering energy barrier CHO intermediate, inducing generation photothermal improves sluggish kinetics PCR efficiency, which ascribed transferred that excited into hot CuInS LSPR effect, accelerating adsorbed molecules.

Language: Английский

Interfacial Mediation by Sn And S Vacancies of p‐SnS/n‐ZnIn2S4 for Enhancing Photocatalytic Hydrogen Evolution with New Scheme of Type‐I Heterojunction DOI
Xiaofang Jia, Yue Lu,

Kunrong Du

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(50)

Published: Aug. 27, 2023

Abstract The construction of interfacial electric field (IEF) in semiconductor heterojunction is great significance boosting photocatalytic hydrogen evolution through efficient separation photogenerated charge‐carriers. However, the exploitation IEF type‐I has not been proposed for designing photocatalysts. Herein, based on density functional theory prediction, p ‐SnS with different work functions modulated by Sn‐vacancy are compounded n ‐ZnIn 2 S 4 containing S‐vacancy to form heterojunction. optimized SnS/ZnIn photocatalyst without co‐catalysts exhibits an impressive rate 22.75 mmol g −1 h , 6.23 times ZnIn . Systematic investigations reveal that Sn‐S bond acts as a transport channel accelerates interface charge‐carriers transfer under promotion originating from significant Fermi level difference. A large difference surface photovoltage signal and achieved effective IEF. new p‐n scheme induced mediation can separate charge‐carriers, retain highly reductive electrons evolution, overcoming disadvantage reduction potential decline typical scheme. This study will afford theoretical basis achievement high‐efficiency modulation.

Language: Английский

Citations

67

Regulating the Metallic Cu–Ga Bond by S Vacancy for Improved Photocatalytic CO2 Reduction to C2H4 DOI
Junyan Wang, Chen Yang, Liang Mao

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(28)

Published: April 20, 2023

Abstract Artificial photosynthesis, which converts carbon dioxide into hydrocarbon fuels, is a promising strategy to overcome both global warming and energy crisis. Herein, the geometric position of Cu Ga on ultra‐thin CuGaS 2 /Ga S 3 oriented via sulfur defect engineering, unprecedented C H 4 yield selectivity ≈93.87% ≈335.67 µmol g −1 h . A highly delocalized electron distribution intensity induced by vacancy indicates that adjacent form Cu–Ga metallic bond, accelerates photocatalytic reduction CO The stability crucial intermediates (*CHOHCO) attributed upshift d ‐band center CGS/GS. C–C coupling barrier intrinsically reduced dominant exposed atoms 2D in process reduction, captures *CO molecules effectively. This study proposes new design photocatalyst through engineering adjust reduction.

Language: Английский

Citations

56

Regulating the Transfer of Photogenerated Carriers for Photocatalytic Hydrogen Evolution Coupled with Furfural Synthesis DOI

Boxin Liu,

Yanfang Li,

Yu-Chen Guo

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(27), P. 17939 - 17949

Published: June 25, 2024

How to simultaneously utilize photogenerated electrons and holes still remains a critical challenge in the field of artificial photosynthesis, especially process photocatalytic hydrogen (H2) evolution coupled with biomass oxidation value-added chemicals. Herein, series-parallel photocatalyst (Cu NPs/CdS/In2O3) that can intrinsically regulate transfer carriers is ingeniously designed for H2 synergized furfural alcohol (FFA) selective (FF). Accordingly, desired FF rates near 100% selectivity toward are achieved on Cu NPs/CdS/In2O3 sealed atmospheric system. Experimental theoretical analyses confirm localized surface plasmon resonance (LSPR) effect induced by NPs accelerates reduction protons (H+) efficiently, while from In2O3 preferentially activate α-C–H bond FFA adsorbed Lewis acid sites generate FF. This work provides reference regulating synthesis.

Language: Английский

Citations

20

Modulating electronic structure and sulfur p-band center by anchoring amorphous Ni@NiSx on crystalline CdS for expediting photocatalytic H2 evolution DOI
Xinlei Zhang, Fei Wu, Guicun Li

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123398 - 123398

Published: Oct. 17, 2023

Language: Английский

Citations

35

Disruption Symmetric Crystal Structure Favoring Photocatalytic CO2 Reduction: Reduced *COOH Formation Energy Barrier on Al Doped CuS/TiO2 DOI
Junyan Wang, Haoyu Zhang, Yao Nian

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: June 24, 2024

Abstract How to break the C═O bond and reduce energy barrier of *COOH formation is key triggering photocatalytic CO 2 reduction (PCR) reaction subsequent proton‐electron processes, which as important overcoming high recombination rate photocarriers. In order solve this issue, symmetric structure CuS/TiO destroyed by S vacancy Al doping (denoted Al‐CuS/TiO ), significantly expands electron localization range promotes cis‐coordination splitting Cu 3 d orbits. The experimental results show that yield selectivity ≈90.68% ≈335.68 µmol·g −1 ·h on . redistribution states in specific / s p orbitals increases adsorption reduces intermediates, while effectively breaking bond. Doped atoms also serve sites for H O molecules, interleaving competition with at staggered. This study provides a new approach accelerate photocarrier migration destroying local symmetry adjust crystal structure, further improving activity PCR.

Language: Английский

Citations

16

Reinforced Interfacial Cd─Se Bond Coupling Photocatalytic Hydrogen Evolution with Pyruvic Acid Synthesis DOI

Yu-Chen Guo,

Jiaming Sun, Zikang Geng

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(32)

Published: May 28, 2024

Abstract Maximizing the utilization of photogenerated electrons and holes to drive coupling reaction hydrogen evolution with selective value‐added organic synthesis holds great potential for more efficient exploitation solar energy. Herein, interstitial boron‐doped CdS is synthesized by taking SiO 2 as a template well adsorption sites boric acid, which contributes boron doping induces reinforced Cd─Se bonding enhancing interfacial interaction co‐catalyst MoSe . Thus, bond electron localization provides rapid channels at atomic level accelerating charge transfer lower energy barrier, achieving high selectivity pyruvic acid concurrently. This work new perspective in avoiding use sacrificial agents uneconomically producing green high‐value‐added chemicals simultaneously.

Language: Английский

Citations

14

All‐in‐One: Plasmonic Janus Heterostructures for Efficient Cooperative Photoredox Catalysis DOI
Chuang Han,

Zikang Zeng,

Xiaorui Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(38)

Published: July 3, 2024

Janus heterostructures consisting of multiple jointed components with distinct properties have gained growing interest in the photoredox catalytic field. Herein, we developed a facile low-temperature method to gain anisotropic one-dimensional Au-tipped CdS (Au-CdS) nanorods (NRs), followed by assembling Ru molecular co-catalyst (RuN

Language: Английский

Citations

12

Photothermal Effect of Cu NCs on CdS Homojunction Boosting Hydrogen Evolution in Alkaline Seawater DOI
Yuan Tang, Yan Sun, Yanfang Li

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(40)

Published: June 27, 2024

Abstract Developing photocatalysts with desired activity and stability toward hydrogen evolution reaction (HER) in alkaline seawater is of prime significance but still pressingly challenging. Herein, cuprum nanoclusters (CuNCs) are anchored on the surface cadmium sulphide homojunctions (CdS‐H) unsaturated edge sulphur (S) by an situ photoreduction technique, which promotes photocatalyst process (H 2 ) (15.5 mmol g −1 h apparent quantum yield 11.0% at 450.0 nm. It comprehensively confirmed that S not only effectively Cu NCs also promoted adsorption chloride ion (Cl − ions, suppressed oxidation lattice modulated seawater. The photothermal effect induced accelerated kinetics, directional migration photocarrier metal‐semiconductor interface demonstrated via method. This work affords a new perspective to rational design high superior performance

Language: Английский

Citations

11

Plasmonic tandem heterojunctions enable high-efficiency charge transfer for broad spectrum photocatalytic hydrogen production DOI
Wenxuan Chen, Xiu-Qing Qiao,

Guohui

et al.

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 1, 2024

Language: Английский

Citations

10

Bifunctional CdS-MoO2 catalysts for selective oxidation of lactic acid coupled with photocatalytic H2 production DOI
Wei Cai, Jincheng Liu,

Yijun Luo

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 675, P. 836 - 847

Published: July 10, 2024

Language: Английский

Citations

9