Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis DOI

Zhi-Sang Huang,

Yinfeng Wang, Ming–Yu Qi

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(47)

Published: Aug. 13, 2024

Abstract Photo‐driven cross‐coupling of o ‐arylenediamines and alcohols has emerged as an alternative for the synthesis bio‐active benzimidazoles. However, tackling key problem related to efficient adsorption activation both coupling partners over photocatalysts towards activity enhancement remains a challenge. Here, we demonstrate interface synergy strategy by exposed oxygen vacancies (V O ) Pd Lewis acid sites benzimidazole hydrogen (H 2 coproduction Pd‐loaded TiO nanospheres with highest photoredox compared previous works so far. The results show that introduction V optimizes energy band structure supplies coordinatively unsaturated adsorbing activating ethanol molecules, affording acetaldehyde active intermediates. acts site, enhancing alkaline amine molecules via acid‐base pair interactions driving condensation process. Furthermore, synergistically promote interfacial charge transfer separation. This work offers new insightful guidance rational design semiconductor‐based at molecular level high‐performance renewable fuels value‐added feedstocks.

Language: Английский

Metal Sulfide S‐Scheme Homojunction for Photocatalytic Selective Phenylcarbinol Oxidation DOI Creative Commons
Huijun Zhang, Yujie Gao, Sugang Meng

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(17)

Published: Feb. 28, 2024

Abstract Metal sulfide‐based homojunction photocatalysts are extensively explored with improved photocatalytic performance. However, the construction of metal S‐scheme remains a challenge. Herein, fabrication 2D CdIn 2 S 4 nanosheets coated 3D octahedra (referred to as 2D/3D n‐CIS/o‐CIS) photocatalyst is reported by simply adjustment polyvinyl pyrrolidone amount during solvothermal synthesis. The formation within n‐CIS/o‐CIS systematically investigated via series characterizations, which can generate an internal electric field facilitate separation and migration photogenerated electron‐hole pairs. composite exhibits significantly activity stability in selective oxidation phenylcarbinol (PhCH OH) benzaldehyde (PhCHO) when compared pure n‐CIS o‐CIS samples under visible light irradiation. It hoped that this work contribute novel insights into development sulfides for solar energy conversion.

Language: Английский

Citations

101
Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis DOI Open Access

Zhi-Sang Huang,

Yinfeng Wang, Ming–Yu Qi

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(47)

Published: Aug. 13, 2024

Abstract Photo‐driven cross‐coupling of o ‐arylenediamines and alcohols has emerged as an alternative for the synthesis bio‐active benzimidazoles. However, tackling key problem related to efficient adsorption activation both coupling partners over photocatalysts towards activity enhancement remains a challenge. Here, we demonstrate interface synergy strategy by exposed oxygen vacancies (V O ) Pd Lewis acid sites benzimidazole hydrogen (H 2 coproduction Pd‐loaded TiO nanospheres with highest photoredox compared previous works so far. The results show that introduction V optimizes energy band structure supplies coordinatively unsaturated adsorbing activating ethanol molecules, affording acetaldehyde active intermediates. acts site, enhancing alkaline amine molecules via acid‐base pair interactions driving condensation process. Furthermore, synergistically promote interfacial charge transfer separation. This work offers new insightful guidance rational design semiconductor‐based at molecular level high‐performance renewable fuels value‐added feedstocks.

Language: Английский

Citations

45
Efficient Photoredox Co-Upcycling of CO2 and Plastic Waste by Band-Gap-Engineered ZnxCd1–xS Catalyst DOI
Yi Zhang, Ming–Yu Qi, Marco Conte

et al.

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 7(1), P. 359 - 367

Published: Dec. 24, 2024

Solar-driven CO2 reduction combined with plastic waste valorization presents a versatile approach to simultaneously reset misaligned hydrocarbon resources and achieve carbon-neutral cycle. Herein, we demonstrate co-upcycling heterogeneous photoredox catalysis for efficient tunable syngas, integrated polyethylene terephthalate (PET) conversion accessing acetate, over the spherical band-gap-engineered ZnxCd1–xS catalyst. The key steering syngas H2/CO rate is modulate conduction band bottom potentials of photocatalysts by altering Zn/Cd ratio, which results in production wide range. Moreover, controlled variations molar ratio regulate electron–hole separation capability, thereby endowing Zn0.8Cd0.2S optimum acetate rates. underlying mechanistic origin such redox reaction involving CO2-assisted PET has been systematically investigated. This win-win cooperative offers tantalizing possibility into value-added feedstocks.

Language: Английский

Citations

29
Enhanced Spin‐Polarized Electric Field Modulating p‐Band Center on Ni‐Doped CdS for Boosting Photocatalytic Hydrogen Evolution DOI
Fei Wu, Xinlei Zhang, Lei Wang

et al.

Small, Journal Year: 2024, Volume and Issue: 20(27)

Published: Jan. 24, 2024

It is a challenge to regulate charge separation dynamics and redox reaction kinetics at the atomic level synergistically boost photocatalytic hydrogen (H

Language: Английский

Citations

24
Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane DOI
Yinfeng Wang, Ming–Yu Qi, Marco Conte

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(34)

Published: June 11, 2024

Abstract Light‐driven photoredox catalysis presents a promising approach for the activation and conversion of methane (CH 4 ) into high value‐added chemicals under ambient conditions. However, C−H bond dissociation energy CH absence well‐defined sites on catalysts significantly limit highly efficient toward multicarbon (C 2+ hydrocarbons, particularly ethylene 2 H ). Herein, we demonstrate bimetallic design Ag nanoparticles (NPs) Pd single atoms (SAs) ZnO cascade C with highest production rate compared previous works. Mechanistic studies reveal that synergistic effect NPs SAs, upon effecting key bond‐breaking ‐forming events, lowers overall barrier process both resulting 6 , constituting truly catalytic system to facilitate generation. This work offers novel perspective advancement photocatalytic directional hydrocarbons through subtle catalyst strategy.

Language: Английский

Citations

20
Tailoring the catalytic sites by regulating photogenerated electron/hole pairs separation spatially for simultaneous selective oxidation of benzyl alcohol and hydrogen evolution DOI
Lifang Yang, Jiao Guo, Siyan Chen

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 659, P. 776 - 787

Published: Jan. 9, 2024

Language: Английский

Citations

17
Multi-channel charge transfer in self-supporting B-g-C3Nx/Bi2S3/CdS dual S-scheme heterojunction toward enhanced photothermal-photocatalytic performance DOI
Yawei Xiao, Mengyao Li, Haoyu Li

et al.

Nano Energy, Journal Year: 2023, Volume and Issue: 120, P. 109164 - 109164

Published: Dec. 5, 2023

Language: Английский

Citations

39
Pauling‐Type Adsorption of O2 Induced by Heteroatom Doped ZnIn2S4 for Boosted Solar‐Driven H2O2 Production DOI

Kailian Zhang,

Lei Tian,

Jingfei Yang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(5)

Published: Dec. 12, 2023

Abstract Breaking the trade‐off between activity and selectivity has perennially been a formidable endeavor in field of hydrogen peroxide (H 2 O ) photosynthesis, especially side‐on configuration oxygen (O on catalyst surface will cause cleavage O−O bonds, which drastically hinders H production performance. Herein, we present an atomically heteroatom P doped ZnIn S 4 with tunable adsorption to accelerate ORR kinetics essential for solar‐driven production. Indeed, spectroscopy characterizations (such as EXAFS situ FTIR) DFT calculations reveal that at substitutional interstitial sites, not only optimizes coordination environment Zn active but also facilitates electron transfer sites improves charge density, avoiding breakage bonds reducing energy barriers As result, is regulated from (Yeager‐type) end‐on (Pauling‐type), resulting accelerated 874.94 2107.66 μmol g −1 h . This finding offers new avenue toward strategic tailoring by rational design photocatalyst.

Language: Английский

Citations

23
Hollow structured CdS@ZnIn2S4 Z-scheme heterojunction for bifunctional photocatalytic hydrogen evolution and selective benzylamine oxidation DOI
Tengfei Bao,

Chenxi Tang,

Shuming Li

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 659, P. 788 - 798

Published: Jan. 6, 2024

Language: Английский

Citations

14
Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane DOI
Yinfeng Wang, Ming–Yu Qi, Marco Conte

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(34)

Published: June 11, 2024

Abstract Light‐driven photoredox catalysis presents a promising approach for the activation and conversion of methane (CH 4 ) into high value‐added chemicals under ambient conditions. However, C−H bond dissociation energy CH absence well‐defined sites on catalysts significantly limit highly efficient toward multicarbon (C 2+ hydrocarbons, particularly ethylene 2 H ). Herein, we demonstrate bimetallic design Ag nanoparticles (NPs) Pd single atoms (SAs) ZnO cascade C with highest production rate compared previous works. Mechanistic studies reveal that synergistic effect NPs SAs, upon effecting key bond‐breaking ‐forming events, lowers overall barrier process both resulting 6 , constituting truly catalytic system to facilitate generation. This work offers novel perspective advancement photocatalytic directional hydrocarbons through subtle catalyst strategy.

Language: Английский

Citations

13