Electron‐Rich Bi Nanosheets Promote CO2⋅− Formation for High‐Performance and pH‐Universal Electrocatalytic CO2 Reduction DOI

Zaiqi Li,

Bin Sun,

Difei Xiao

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(11)

Published: Jan. 20, 2023

Electrochemical CO2 reduction reaction (CO2 RR) to chemical fuels such as formate offers a promising pathway carbon-neutral future, but its practical application is largely inhibited by the lack of effective activation molecules and pH-universal feasibility. Here, we report an electronic structure manipulation strategy electron-rich Bi nanosheets, where electrons transfer from Cu donor acceptor in bimetallic Cu-Bi, enabling RR towards with concurrent high activity, selectivity stability (acidic, neutral alkaline) electrolytes. Combined situ Raman spectra computational calculations unravel that promotes ⋅- formation activate molecules, enhance adsorption strength *OCHO intermediate up-shifted p-band center, thus leading superior activity formate. Further integration robust nanosheets into III-V-based photovoltaic solar cell results unassisted artificial leaf solar-to-formate (STF) efficiency 13.7 %.

Language: Английский

Strain enhances the activity of molecular electrocatalysts via carbon nanotube supports DOI Creative Commons
Jianjun Su, Charles B. Musgrave, Yun Mi Song

et al.

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(9), P. 818 - 828

Published: Aug. 14, 2023

Abstract Support-induced strain engineering is useful for modulating the properties of two-dimensional materials. However, controlling planar molecules technically challenging due to their sub-2 nm lateral size. Additionally, effect on molecular remains poorly understood. Here we show that carbon nanotubes (CNTs) are ideal substrates inducing optimum through curvature. In a tandem-flow electrolyser with monodispersed cobalt phthalocyanine (CoPc) single-walled CNTs (CoPc/SWCNTs) CO 2 reduction, achieve methanol partial current density >90 mA cm −2 >60% selectivity, surpassing wide multiwalled at 16.6%. We report vibronic and X-ray spectroscopies unravel distinct local geometries electronic structures induced by strong molecule–support interactions. Grand canonical functional theory confirms curved CoPc/SWCNTs improve *CO binding enable subsequent whereas favour desorption. Our results important role SWCNTs beyond catalyst dispersion electron conduction.

Language: Английский

Citations

219
Defect engineering of two-dimensional materials for advanced energy conversion and storage DOI
Fu Liu, Zhanxi Fan

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(5), P. 1723 - 1772

Published: Jan. 1, 2023

Defective two-dimensional (2D) materials show huge potential for energy-related fields. This review overviews the formation/evolution mechanisms and engineering strategies of defects in 2D materials, which enable enhanced electrode reaction kinetics.

Language: Английский

Citations

211
Design strategies for markedly enhancing energy efficiency in the electrocatalytic CO2 reduction reaction DOI
Wenchuan Lai, Yan Qiao, Jiawei Zhang

et al.

Energy & Environmental Science, Journal Year: 2022, Volume and Issue: 15(9), P. 3603 - 3629

Published: Jan. 1, 2022

The review summarizes the recent strategies to improve energy efficiency of CO 2 electroreduction, a guiding metric for industrial application and economic feasibility, with emphasis on designing remarkable catalyst advanced electrolysis system.

Language: Английский

Citations

200
Electrochemical reduction of carbon dioxide to multicarbon (C2+) products: challenges and perspectives DOI Creative Commons
Bin Chang, Hong Pang,

Fazal Raziq

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(11), P. 4714 - 4758

Published: Jan. 1, 2023

This review analyzes advanced catalysts and C 2+ synthesis mechanisms based on theoretical explorations in situ / operando characterizations. Triphasic interface optimization is discussed for the potential of industry-compatible stability.

Language: Английский

Citations

193
CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment DOI Creative Commons

Zesong Ma,

Zhilong Yang, Wenchuan Lai

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Dec. 9, 2022

Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect cation synergistically modulate local microenvironment. A Faradaic efficiency 83.7 ± 1.4% partial current density 0.56 0.02 cm-2, single-pass carbon 54.4%, stable electrolysis 30 h a flow cell are demonstrated for aqueous consisting sulfuric acid KCl with pH 1. Mechanistically, accumulated species (e.g., K+ OH-) Helmholtz plane account selectivity activity toward kinetically reducing proton coverage thermodynamically favoring conversion. We find that cations facilitate C-C coupling through interaction between key intermediate *OCCO.

Language: Английский

Citations

181
Conversion of CO2 to multicarbon products in strong acid by controlling the catalyst microenvironment DOI
Yong Zhao, Long Hao, Adnan Ozden

et al.

Nature Synthesis, Journal Year: 2023, Volume and Issue: unknown

Published: Feb. 9, 2023

Language: Английский

Citations

170
Durable CO2 conversion in the proton-exchange membrane system DOI

Wensheng Fang,

Wei Guo, Ruihu Lu

et al.

Nature, Journal Year: 2024, Volume and Issue: 626(7997), P. 86 - 91

Published: Jan. 31, 2024

Language: Английский

Citations

164
Challenges and Opportunities in Electrocatalytic CO2 Reduction to Chemicals and Fuels DOI Creative Commons
Xiaojie She, Yifei Wang, Hui Xu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(49)

Published: Aug. 22, 2022

The global temperature increase must be limited to below 1.5 °C alleviate the worst effects of climate change. Electrocatalytic CO

Language: Английский

Citations

158
2022 roadmap on low temperature electrochemical CO2 reduction DOI Creative Commons
Ifan E. L. Stephens, Karen Chan, Alexander Bagger

et al.

Journal of Physics Energy, Journal Year: 2022, Volume and Issue: 4(4), P. 042003 - 042003

Published: June 13, 2022

Abstract Electrochemical CO 2 reduction (CO R) is an attractive option for storing renewable electricity and the sustainable production of valuable chemicals fuels. In this roadmap, we review recent progress in fundamental understanding, catalyst development, engineering scale-up. We discuss outstanding challenges towards commercialization electrochemical R technology: energy efficiencies, selectivities, low current densities, stability. highlight opportunities establishing rigorous standards benchmarking performance, advances operando characterization, discovery new materials high value products, investigation phenomena across multiple-length scales application data science doing so. hope that collective perspective sparks research activities ultimately bring us a step closer low- or zero-emission carbon cycle.

Language: Английский

Citations

157
Enrichment of reactants and intermediates for electrocatalytic CO2reduction DOI
Peng‐Peng Yang, Min‐Rui Gao

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(13), P. 4343 - 4380

Published: Jan. 1, 2023

The electrocatalytic carbon dioxide reduction reaction (CO2RR) presents a sustainable route to convert renewable electricity value-added fuels and feedstocks in the form of chemical energy. However, selectivity rate conversion CO2 desirable carbon-based products, especially multicarbon remain below requirement for its implementation at commercial scale, which primarily originates from inadequate reactants intermediates near catalytic surfaces during CO2RR. enrichment provides one coping guidelines improve CO2RR performance by accelerating improving product selectivity. Herein, we discuss strategies achieve through catalyst design, local microenvironment modulation, electrolyte regulation, electrolyzer optimization. structure properties are first presented, showing necessity feasibility enriching intermediates. Next, influence effect on electrolysis, i.e., selectivity, comprehensively discussed. Then, design micrometer scale atom including wettability morphology surface modification, tandem construction, as well engineering, is highlighted implement Catalyst restructuring process impact also Subsequently, modulating high utilization produce products reviewed. After that, insights into regulation provided investigating various electrolytes, aqueous solutions, organic solvents, ionic liquids. Additionally, key role optimization promoting considered. We end review outlining remaining technological challenges providing feasible suggestions aimed directing future employment propel practical electrolysis technology.

Language: Английский

Citations

155