Nanoarchitectonics of Metallene Materials for Electrocatalysis DOI
Bo Jiang, Yanna Guo,

Fengyu Sun

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(14), P. 13017 - 13043

Published: June 27, 2023

Controlling the synthesis of metal nanostructures is one approach for catalyst engineering and performance optimization in electrocatalysis. As an emerging class unconventional electrocatalysts, two-dimensional (2D) metallene electrocatalysts with ultrathin sheet-like morphology have gained ever-growing attention exhibited superior electrocatalysis owing to their distinctive properties originating from structural anisotropy, rich surface chemistry, efficient mass diffusion capability. Many significant advances synthetic methods electrocatalytic applications 2D metallenes been obtained recent years. Therefore, in-depth review summarizing progress developing electrochemical highly needed. Unlike most reported reviews on metallenes, this starts by introducing preparation based classification metals (e.g., noble metals, non-noble metals) instead methods. Some typical strategies preparing each kind are enumerated detail. Then, utilization applications, especially conversion reactions, including hydrogen evolution reaction, oxygen reduction fuel oxidation CO2 N2 comprehensively discussed. Finally, current challenges opportunities future research energy proposed.

Language: Английский

Mechanistic Insights into OC–COH Coupling in CO2 Electroreduction on Fragmented Copper DOI
Kaili Yao, Jun Li, Haibin Wang

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(31), P. 14005 - 14011

Published: July 29, 2022

The carbon–carbon (C–C) bond formation is essential for the electroconversion of CO2 into high-energy-density C2+ products, and precise coupling pathways remain controversial. Although recent computational investigations have proposed that OC–COH pathway more favorable in specific reaction conditions than well-known CO dimerization pathway, experimental evidence still lacking, partly due to separated catalyst design mechanistic/spectroscopic exploration. Here, we employ density functional theory calculations show on low-coordinated copper sites, *CO bindings are strengthened, adsorbed with their hydrogenation species, *COH, receives precedence over dimerization. Experimentally, construct a fragmented Cu abundant exhibiting 77.8% Faradaic efficiency products at 300 mA cm–2. With suite situ spectroscopic studies, capture an *OCCOH intermediate surfaces, providing direct support pathway. mechanistic insights this research elucidate how materials favor toward efficient production from reduction.

Language: Английский

Citations

129
A Nanocomposite of Bismuth Clusters and Bi2O2CO3 Sheets for Highly Efficient Electrocatalytic Reduction of CO2 to Formate DOI
Lin Li, Xiaoyang He, Xia‐Guang Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(3)

Published: Oct. 29, 2022

The renewable-electricity-driven CO2 reduction to formic acid would contribute establishing a carbon-neutral society. current catalyst suffers from limited activity and stability under high selectivity the ambiguous nature of active sites. Herein, we report powerful Bi2 S3 -derived that demonstrates density 2.0 A cm-2 with formate Faradaic efficiency 93 % at -0.95 V versus reversible hydrogen electrode. energy conversion single-pass yield reach 80 67 %, respectively, durability reaches 100 h an industrial-relevant density. Pure concentration 3.5 mol L-1 has been produced continuously. Our operando spectroscopic theoretical studies reveal dynamic evolution into nanocomposite composed Bi0 clusters O2 CO3 nanosheets pivotal role -Bi2 interface in activation conversion.

Language: Английский

Citations

110
In-situ spectroscopic probe of the intrinsic structure feature of single-atom center in electrochemical CO/CO2 reduction to methanol DOI Creative Commons

Xinyi Ren,

Jian Zhao,

Xuning Li

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 9, 2023

While exploring the process of CO/CO2 electroreduction (COxRR) is great significance to achieve carbon recycling, deciphering reaction mechanisms so as further design catalytic systems able overcome sluggish kinetics remains challenging. In this work, a model single-Co-atom catalyst with well-defined coordination structure developed and employed platform unravel underlying mechanism COxRR. The as-prepared exhibits maximum methanol Faradaic efficiency high 65% at 30 mA/cm2 in membrane electrode assembly electrolyzer, while on contrary, reduction pathway CO2 strongly decreased CO2RR. In-situ X-ray absorption Fourier-transform infrared spectroscopies point different adsorption configuration *CO intermediate CORR compared that CO2RR, weaker stretching vibration C-O bond former case. Theoretical calculations evidence low energy barrier for formation H-CoPc-CO- species, which critical factor promoting electrochemical CO methanol.

Language: Английский

Citations

110
Designing Cu-Based Tandem Catalysts for CO2 Electroreduction Based on Mass Transport of CO Intermediate DOI
Bo Cao, Fuzhi Li, Jun Gu

et al.

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(15), P. 9735 - 9752

Published: July 27, 2022

Electrochemical reduction of CO2 to high-value hydrocarbons and oxygenates is an attractive technique store intermittent renewable energy. Diverse catalysts are capable catalyzing the CO conversion, while further occurs almost exclusively on Cu. Monocomponent Cu suffer from high overpotential low Faradaic efficiency oxygenates. Combining conversion Au, Ag, single-atom catalysts, etc., with a promising strategy achieve selectivity formation rate highly reduced products. Numerous tandem have been developed based this idea, mass transport intermediate CO-formation catalyst key factor that needs be considered in design catalysts. Rational analysis different modes reported designs needed for development reduction. In review, we elucidate how spatial distribution determines mode consequently affects utilization intermediate. We also discuss challenges perspectives understanding interaction between improving their catalytic performance

Language: Английский

Citations

109
Selective CO2 electrolysis to CO using isolated antimony alloyed copper DOI Creative Commons
Jiawei Li, Hongliang Zeng, Xue Dong

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Jan. 20, 2023

Abstract Renewable electricity-powered CO evolution from 2 emissions is a promising first step in the sustainable production of commodity chemicals, but performing electrochemical reduction economically at scale challenging since only noble metals, for example, gold and silver, have shown high performance -to-CO. Cu potential catalyst to achieve industrial scale, C-C coupling process on significantly depletes CO* intermediates, thus limiting rate producing many hydrocarbon oxygenate mixtures. Herein, we tune selectivity by alloying second metal Sb into Cu, report an antimony-copper single-atom alloy (Sb 1 Cu) isolated Sb-Cu interfaces that catalyzes efficient conversion -to-CO with Faradaic efficiency over 95%. The partial current density reaches 452 mA cm −2 approximately 91% efficiency, negligible C 2+ products are observed. In situ spectroscopic measurements theoretical simulations reason atomic interface promotes adsorption/activation weakens binding strength CO*, which ends up enhanced rates.

Language: Английский

Citations

109
Tailoring acidic microenvironments for carbon-efficient CO2electrolysis over a Ni–N–C catalyst in a membrane electrode assembly electrolyzer DOI
Hefei Li, Haobo Li, Pengfei Wei

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(4), P. 1502 - 1510

Published: Jan. 1, 2023

By tailoring the microenvironments of a Ni–N–C catalyst in an acidic MEA electrolyzer, we achieve CO faradaic efficiency 95% at 500 mA cm −2 , and 2 loss is reduced by 86% 300 pH 0.5, compared to alkaline electrolysis.

Language: Английский

Citations

109
Understanding and leveraging the effect of cations in the electrical double layer for electrochemical CO2 reduction DOI Creative Commons
Binbin Pan, Yuhang Wang, Yanguang Li

et al.

Chem Catalysis, Journal Year: 2022, Volume and Issue: 2(6), P. 1267 - 1276

Published: April 18, 2022

Language: Английский

Citations

104
Multicarbons generation factory: CuO/Ni single atoms tandem catalyst for boosting the productivity of CO2 electrocatalysis DOI
Yu Zhang, Peng Li, Changming Zhao

et al.

Science Bulletin, Journal Year: 2022, Volume and Issue: 67(16), P. 1679 - 1687

Published: July 28, 2022

Language: Английский

Citations

102
In situ Raman spectroscopy studies for electrochemical CO2 reduction over Cu catalysts DOI
Hefei Li, Pengfei Wei, Dunfeng Gao

et al.

Current Opinion in Green and Sustainable Chemistry, Journal Year: 2022, Volume and Issue: 34, P. 100589 - 100589

Published: Jan. 8, 2022

Language: Английский

Citations

101
Membrane Electrode Assembly for Electrocatalytic CO2 Reduction: Principle and Application DOI
Zheng Zhang, Xin Huang, Zhou Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(28)

Published: March 27, 2023

Abstract Electrocatalytic CO 2 reduction reaction (CO RR) in membrane electrode assembly (MEA) systems is a promising technology. Gaseous can be directly transported to the cathode catalyst layer, leading enhanced rate. Meanwhile, there no liquid electrolyte between and anode, which help improve energy efficiency of whole system. The remarkable progress achieved recently points out way realize industrially relevant performance. In this review, we focus on principles MEA for RR, focusing gas diffusion electrodes ion exchange membranes. Furthermore, anode processes beyond oxidation water are considered. Besides, voltage distribution scrutinized identify specific losses related individual components. We also summarize generation different reduced products together with corresponding catalysts. Finally, challenges opportunities highlighted future research.

Language: Английский

Citations

91