Atomic Active Centers Anchored Photocatalysts for CO2 Reduction to Renewable Ethylene/Ethane DOI Creative Commons
Elhussein M. Hashem, Amin Talebian‐Kiakalaieh,

Meijun Guo

et al.

Small Structures, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 26, 2024

Photocatalytic CO 2 reduction to ethylene/ethane offers a sustainable and cost‐effective approach simultaneously produce these high‐demand chemicals while reducing atmospheric level. Lately, atomic active centers (AACs) anchored photocatalysts are comprehensively investigated for their exceptional photocatalytic performance regarding the photosynthesis of ethylene/ethane. This review provides critical summary incorporation various AACs, such as Cu, Au, Ag, Mo, Ni, P/Cu, CuAu, onto different photocatalyst supports, including metal oxide, carbon nitride, red phosphorous, covaleng organic framework , bimetallic sulfide together with crucial role in raising rates production selectivities. Furthermore, this comprehensive summary/analyses preparation routes, chemical composition, configurations, coordination structures, optical characteristics, structure–performance relationship, reaction intermediates, pathways, photocatalysis mechanism, performances as‐prepared AAC using state‐of‐art situ characterization techniques. also emphasizes challenges process conversion target products, limitations, potential applications, future outlooks AACs photocatalysts.

Language: Английский

Precision Molecular Engineering of Carbon Nitride for Efficient and Selective Photoreduction of CO2 to C2H6 in Pure Water DOI Open Access

Zihe Chen,

Guixiang Ding,

Zhaoqiang Wang

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 7, 2025

Abstract Photocatalytic CO 2 reduction into high‐value C 2+ products such as H 6 is of great importance but challenging due to their multi‐electron steps and high energy barrier C─C coupling. Moreover, improving its solar‐to‐chemical (STC) conversion efficiency in pure water beyond the current 1% empirical value also a significant challenge. Herein, graphite carbon nitride (g‐C 3 N 4 ) nanosheets with controllable (C) doping nitrogen (N) vacancies (PCCN‐x) are designed through biochar‐tailored protocol for efficiently selectively photo‐converting . The optimal PCCN‐10 photocatalyst enables achievement an exceptional activity 99.14 µmol g −1 h selectivity 80.33% over 20 water. A record STC ≈1.13% solar fuel production from O vapor achieved without any other inputs. Outdoor tests demonstrated impressive ‐to‐C photo‐conversion rate 43.17 water, stable 50 period. Critically, experimental theoretical calculations further confirm pivotal role bridged sites activating molecules promoting formation coupling intermediate ( * OCCO), which very beneficial performance this work photocatalytic fuels paves way large‐scale broader sustainable applications.

Language: Английский

Citations

5
Ir-O-Mn embedded in porous nanosheets enhances charge transfer in low-iridium PEM electrolyzers DOI Creative Commons
Dawei Wang,

Fangxu Lin,

Heng Luo

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 2, 2025

Using metal oxides to disperse iridium (Ir) in the anode layer proves effective for lowering Ir loading proton exchange membrane water electrolyzers (PEMWE). However, reported low-Ir-based catalysts still suffer from unsatisfying electrolytic efficiency and durability under practical industrial working conditions, mainly due insufficient catalytic activity mass transport catalyst layer. Herein we report a class of porous heterogeneous nanosheet with abundant Ir-O-Mn bonds, achieving notable 4 A mgIr−1 oxygen evolution reaction at an overpotential 300 mV, which is 150.6 times higher than that commercial IrO2. bonds are unraveled serve as efficient charge-transfer channels between in-situ electrochemically-formed IrOx clusters MnOx matrix, fostering generation stabilization highly active Ir3+ species. Notably, Ir/MnOx-based PEMWE demonstrates comparable performance 10-fold lower (0.2 mgIr cm−2), taking low cell voltage 1.63 V deliver 1 cm−2 over h, positions it among elite Ir-based PEMWEs. Building proton-exchange electrolyzer remains important but challenging. Here, authors Ir/MnOx rich generate stabilize species, enhancing both stability.

Language: Английский

Citations

2
Cooperative Atomic Palladium Site and Island-Distributed S-Scheme Heterostructure for Photocatalytic C2H6 Production DOI
Yan Wu, Zhujie Li, Qingqing Chen

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 3558 - 3569

Published: Feb. 12, 2025

Language: Английский

Citations

1
Constructing an Active Sulfur‐Vacancy‐Rich Surface for Selective *CH3‐CH3 Coupling in CO2‐to‐C2H6 Conversion With 92% Selectivity DOI Open Access

Xiaonan Yang,

Liteng Ren,

Zhiheng Chen

et al.

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

Published: Nov. 6, 2024

Abstract To achieve high selectivity in photocatalytic CO 2 reduction to C 2+ products, increasing the number of adsorption sites and lowering energy barriers for key intermediates are critical. A ZnIn S 4 (ZIS)/MoO 3‐x (Z‐M) photocatalyst is presented, which plasmonic MoO generates hot electrons, creating a multielectron environment ZIS that facilitates efficient C─C coupling reactions. Density functional theory (DFT) calculations reveal reduces formation sulfur vacancies (S V ) ZIS, thereby enhancing activation. The ‐rich surface lowers barrier forming HCOO * −0.33 eV whereas COOH 0.77 eV. Successive hydrogenation leads CH , converts 3 with an −0.63 ‐CH 0.54 eV, lower than 0.73 form H . Thus, Z‐M preferentially produces 6 over Under visible light, achieves ‐to‐C conversion rate 467.3 µmol g −1 h 92.0% selectivity. This work highlights dual role photocatalysts improving production reduction.

Language: Английский

Citations

4
Study on the high-efficiency CO2 mineralization reaction mechanism of thermally modified materials from neutralized gypsum residue driven by sulfur vacancies in an aqueous environment DOI

Yuwen Deng,

Sisi Chen, Huidong Tang

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 163591 - 163591

Published: May 1, 2025

Language: Английский

Citations

0
Synergetic Effect of Heterojunction and Sulfur Vacancy on ZnIn2S4/CeO2 to Enhance the Photocatalytic Performance of 5‐Hydroxymethylfurfural into 2,5‐Diformylfuran DOI
Yue Wang, Huai Liu,

Tianping Lv

et al.

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

Published: Oct. 18, 2024

Abstract The efficient separation of photocarriers and facile generation superoxide radicals are crucial for enhancing the performance photocatalysts in selectively photo‐oxidizing 5‐hydroxymethylfurfural (HMF) into 2,5‐diformylfuran (DFF). Herein, a ZnIn 2 S 4 /CeO composite with S‐scheme heterojunction sulfur vacancies (S V ) is successfully developed through one‐step hydrothermal method. optimal catalyst ‐ZnIn exhibits excellent catalytic activity 100% conversion HMF 96.1% selectivity DFF 80 min under ambient conditions, production rate up to 952.6 µmol g −1 h . Intriguingly, remains significant even when concentration increased from 8 100 mм. Experimental theoretical investigations discover that synergistic effect contribute activation oxygen, which facilitate radicals, thus boosting oxidation reactions.

Language: Английский

Citations

2
Computational Screening of Asymmetric Dual Sites by Bader Charge Variation Facilitates C–C Coupling for CO2 Photoreduction to C2H4 DOI
Qian Zhu, Zhiyu Shao, Xinyue Wang

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(47), P. 17336 - 17346

Published: Nov. 12, 2024

Constructing asymmetric dual active sites is an effective strategy to promote formation of the C2 product in photocatalytic CO2 reactions, attributed suppressed dipole–dipole repulsion facilitating C–C coupling. However, information about extent asymmetry still absent, making precise design a challenge. Herein, Bader charge variation (Δq) intermetallics was chosen as descriptor select sites, where linear relation between Δq and adsorption energy intermediate found. From 66 intermetallic candidates, FePt stood out, with = 0.503 e–, predicted be promising candidate. Experimentally, nanoparticles were synthesized loaded onto substrate TiO2 (denoted FePt/TiO2), CoPt NiPt also reference samples. X-ray photoelectron spectroscopy absorption results reveal electron enrichment on Pt depletion Fe, DFT calculations uncover that distribution strengthened intermediate's coupling, reducing free barrier 0.68 eV. As result, FePt/TiO2 showed efficient production C2H4 (4.8 μmol g–1 h–1) absence photosensitizers scavengers, higher than amounts obtained CoPt/TiO2, NiPt/TiO2, (2.1, 1.5, 0 h–1, respectively). This study offers insights into criteria motivate photoreduction.

Language: Английский

Citations

1
Employing facile molten-salt strategy towards erbium ornamentation over CuInS2 for upgrading visible-light-driven hydrogen production and Cr(VI) reduction DOI
Fulin Wang, Yanming Yang, Xiangwei Li

et al.

Journal of environmental chemical engineering, Journal Year: 2024, Volume and Issue: 12(6), P. 114788 - 114788

Published: Nov. 13, 2024

Language: Английский

Citations

1
Anti-Site Defect-Induced Cascaded Sub-Band Transition in CuInS2 Enables Infrared Light-Driven CO2 Reduction DOI
Chen Liao, Zhi-Zhong He, Feng Wang

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(52), P. 35480 - 35489

Published: Dec. 18, 2024

Photocatalytic CO2 conversion is a promising approach to simultaneously mitigate climate change and alleviate the energy crisis. However, infrared light, which constitutes nearly half of solar energy, has not been effectively utilized yet. In this work, we discover photogenerated charge transition mechanism in CuInS2 with intrinsic InCu antisite defects for synergistic utilization full-spectrum photons. Femtosecond transient absorption spectroscopy DFT calculation unveil an intermediate band induced by defects, where cascaded sub-band could be realized high-energy photons (UV–vis) low-energy (IR), thus improving range light as well efficiency carriers. situ Kelvin probe force microscopy demonstrates that generation photoexcited electrons greatly enhanced through full spectrum light. Moreover, X-ray photoelectron diffuse reflectance Fourier transform reveal also enhance adsorption activation H2O on catalyst surface. As result, CO production rate under reaches 19.9 μmol g–1 h–1, more than 7-fold increase over UV–vis irradiation.

Language: Английский

Citations

1
Pt single atoms promoting the construction of asymmetric double sites to achieve highly selective photoreduction of CO2 to ethylene DOI

Jiang Mo,

Su Liu,

Quan‐Qing Xu

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 683, P. 301 - 309

Published: Dec. 20, 2024

Language: Английский

Citations

1