Hybrid Catalyst Coupling Zn Single Atoms and CuNx Clusters for Synergetic Catalytic Reduction of CO2 DOI
Xiao Hu, Xinyu Liu,

Xin Hu

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(16)

Published: Feb. 2, 2023

Abstract Reverse water‐gas shift (RWGS) reaction is the initial and necessary step of CO 2 hydrogenation to high value‐added products, regulating selectivity still a fundamental challenge. In present study, an efficient catalyst (CuZnN x @C‐N) composed by Zn single atoms Cu clusters stabilized nitrogen sites reported. It contains saturated four‐coordinate Zn‐N 4 low valence CuN clusters. Monodisperse induces aggregation pyridinic N form structures, which show strong Lewis basicity has adsorption for *CO *COOH intermediates, but weak *CO, thus greatly improves conversion selectivity. The calcined at 700 °C exhibits highest 43.6% under atmospheric pressure, 18.33 times Cu‐ZnO close thermodynamic equilibrium rate (49.9%) . catalytic process, not only adsorbs activates H , also cooperates with adjacent structures jointly activate molecules further promotes This synergistic mechanism will provide new insights developing catalysts.

Language: Английский

Revolutionizing CO2 Electrolysis: Fluent Gas Transportation within Hydrophobic Porous Cu2O DOI

Qinghong Geng,

Longlong Fan, Huige Chen

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(15), P. 10599 - 10607

Published: April 3, 2024

The success of electrochemical CO2 reduction at high current densities hinges on precise interfacial transportation and the local concentration gaseous CO2. However, creation efficient channels remains an unexplored frontier. In this study, we design synthesize hydrophobic porous Cu2O spheres with varying pore sizes to unveil nanoporous channel's impact gas transfer triple-phase interfaces. not only facilitate rapid but also trap compressed bubbles form abundant stable interfaces, which are crucial for high-current-density electrocatalysis. electrolysis, in situ spectroscopy density functional theory results reveal that atomic edges concave surfaces promote C–C coupling via energetically favorable OC-COH pathway, leading overwhelming CO2-to-C2+ conversion. Leveraging optimal active site exposure, a 240 nm size (P-Cu2O-240) stands out among all samples exhibits best productivity remarkable Faradaic efficiency formation rate up 75.3 ± 3.1% 2518.2 8.1 μmol h–1 cm–2, respectively. This study introduces novel paradigm electrocatalysts concurrently addresses gas-transfer challenges.

Language: Английский

Citations

43
Well-defined diatomic catalysis for photosynthesis of C2H4 from CO2 DOI Creative Commons

Zhongkai Xie,

Shengjie Xu, Longhua Li

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 18, 2024

Abstract Owing to the specific electronic-redistribution and spatial proximity, diatomic catalysts (DACs) have been identified as principal interest for efficient photoconversion of CO 2 into C H 4 . However, predominant bottom-up strategy DACs synthesis has critically constrained development highly ordered due random distribution heteronuclear atoms, which hinders optimization catalytic performance exploration actual reaction mechanism. Here, an up-bottom ion-cutting architecture is proposed fabricate well-defined DACs, superior proximity CuAu diatomics (DAs) decorated TiO (CuAu-DAs-TiO ) successfully constructed compact heteroatomic spacing (2-3 Å). profoundly low C-C coupling energy barrier CuAu-DAs-TiO , a considerable production with sustainability achieved. Our discovery inspires novel fabrication motivate distinct deduction heteroatom synergistically

Language: Английский

Citations

42
Lattice Oxygen Activation through Deep Oxidation of Co4N by Jahn–Teller–Active Dopants for Improved Electrocatalytic Oxygen Evolution DOI
Jingrui Han, Haibin Wang, Yuting Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(33)

Published: May 27, 2024

Triggering the lattice oxygen oxidation mechanism is crucial for improving evolution reaction (OER) performance, because it could bypass scaling relation limitation associated with conventional adsorbate through direct formation of oxygen-oxygen bond. High-valence transition metal sites are favorable activating oxygen, but deep pre-catalysts suffers from a high thermodynamic barrier. Here, taking advantage Jahn-Teller (J-T) distortion induced structural instability, we incorporate high-spin Mn

Language: Английский

Citations

42
Low‐coordination Nanocrystalline Copper‐based Catalysts through Theory‐guided Electrochemical Restructuring for Selective CO2 Reduction to Ethylene DOI

Wensheng Fang,

Ruihu Lu, Fumin Li

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(16)

Published: Feb. 19, 2024

Revealing the dynamic reconstruction process and tailoring advanced copper (Cu) catalysts is of paramount significance for promoting conversion CO

Language: Английский

Citations

38
In situ copper faceting enables efficient CO2/CO electrolysis DOI Creative Commons
Kaili Yao, Jun Li, Adnan Ozden

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 26, 2024

Abstract The copper (Cu)-catalyzed electrochemical CO 2 reduction provides a route for the synthesis of multicarbon (C 2+ ) products. However, thermodynamically favorable Cu surface (i.e. Cu(111)) energetically favors single-carbon production, leading to low energy efficiency and production rates C Here we introduce in situ faceting from enable preferential exposure Cu(100) facets. During precatalyst evolution, phosphate ligand slows assists generation co-adsorption hydroxide ions, steering reconstruction (100). resulting catalyst enables current densities > 500 mA cm −2 Faradaic efficiencies >83% towards products both reduction. When run at 150 hours, maintains 37% full-cell 95% single-pass carbon throughout.

Language: Английский

Citations

31
Cooperation of Different Active Sites to Promote CO2 Electroreduction to Multi‐carbon Products at Ampere‐Level DOI

Dawei Zhou,

Chunjun Chen, Yichi Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 12, 2024

Abstract Electroreduction of CO 2 to C 2+ products provides a promising strategy for reaching the goal carbon neutrality. However, achieving high selectivity at current density remains challenge. In this work, we designed and prepared multi‐sites catalyst, in which Pd was atomically dispersed Cu (Pd−Cu). It found that Pd−Cu catalyst had excellent performance producing from electroreduction. The Faradaic efficiency (FE) could be maintained approximately 80.8 %, even 0.8 A cm −2 least 20 hours. addition, FE above 70 % 1.4 . Experiments functional theory (DFT) calculations revealed three distinct catalytic sites. These active sites allowed efficient conversion , water dissociation, conversion, ultimately leading yields products.

Language: Английский

Citations

29
Low-coordinated copper facilitates the *CH2CO affinity at enhanced rectifying interface of Cu/Cu2O for efficient CO2-to-multicarbon alcohols conversion DOI Creative Commons
Yangyang Zhang, Yanxu Chen, Xiaowen Wang

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 18, 2024

Abstract The carbon−carbon coupling at the Cu/Cu 2 O Schottky interface has been widely recognized as a promising approach for electrocatalytic CO conversion into value-added alcohols. However, limited selectivity of C 2+ alcohols persists due to insufficient control over rectifying characteristics required precise bonding oxyhydrocarbons. Herein, we present an investigation manipulation coordination environment Cu sites through in-situ electrochemical reconstruction strategy, which indicates that construction low-coordinated facilitates enhanced interfaces, and induces asymmetric electronic perturbation faster electron exchange, thereby boosting C-C oxyhydrocarbons towards nucleophilic reaction process *H CCO-CO. Impressively, exhibit superior faradic efficiency 64.15 ± 1.92% energy ~39.32% production, while maintaining stability 50 h (faradic >50%, total current density = 200 mA cm −2 ) in flow-cell electrolyzer. Theoretical calculations, operando synchrotron radiation Fourier transform infrared spectroscopy, Raman experiments decipher can enhance coverage *CO adsorption *CH CH CHO, facilitating formation

Language: Английский

Citations

29
Doping engineering of Cu-based catalysts for electrocatalytic CO2 reduction to multi-carbon products DOI

Shiya You,

Jiewen Xiao, Shuyu Liang

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(16), P. 5795 - 5818

Published: Jan. 1, 2024

Recent developments in heteroatom-doped Cu-based catalysts for CO 2 electroreduction into C 2+ products are highlighted. The design strategies doped and situ technologies discussed.

Language: Английский

Citations

29
Selective Electrosynthesis of Ethanol via Asymmetric C–C Coupling in Tandem CO2 Reduction DOI

Peng Luan,

Xue Dong, Linqi Liu

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8776 - 8785

Published: May 21, 2024

Selective electroreduction of CO2 to ethanol has economic value and environmental significance. However, the activity selectivity reduction toward are still low due sluggish kinetics C–C coupling intense competition hydrocarbon production. Herein, we report a layered tandem catalyst consisting Cu nanosheets with Cu(111)-oriented surface Ag nanoparticles, which can effectively shift from hydrocarbons ethanol. The Faradaic efficiency was improved less than 30% on bare Cu(111) 56.5 ± 2.6% Cu/Ag catalysts, partial current density 356.7 9.5 mA cm–2. In situ Raman spectroscopy results functional theory calculations suggest that high be attributed asymmetric *CH2–CO mechanism, is facilitated by selective generation *CH2 species (111)-facet-exposed local CO concentration supplied catalyst.

Language: Английский

Citations

21
Nanocavity enriched CuPd alloy with high selectivity for CO2 electroreduction toward C2H4 DOI
Ze-Yu Zhang, Haibin Wang,

Fei-Fei Zhang

et al.

Rare Metals, Journal Year: 2024, Volume and Issue: 43(4), P. 1513 - 1523

Published: Jan. 20, 2024

Language: Английский

Citations

19