Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites DOI Creative Commons
Le Li, Adnan Ozden, Shuyi Guo

et al.

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Sept. 1, 2021

Abstract Electrochemical reduction of CO 2 (CO R) to formic acid upgrades waste ; however, up now, chemical and structural changes the electrocatalyst have often led deterioration performance over time. Here, we find that alloying p-block elements with differing electronegativities modulates redox potential active sites stabilizes them throughout extended R operation. Active Sn-Bi/SnO surfaces formed in situ on homogeneously alloyed Bi 0.1 Sn crystals stabilize R-to-formate pathway 2400 h (100 days) continuous operation at a current density 100 mA cm −2 . This is accompanied by Faradaic efficiency 95% an overpotential ~ −0.65 V. Operating experimental studies as well computational investigations show stabilized offer near-optimal binding energy key formate intermediate *OCHO. Using cation-exchange membrane electrode assembly device, demonstrate stable production concentrated HCOO – solution (3.4 molar, 15 wt%) h.

Language: Английский

Technologies and perspectives for achieving carbon neutrality DOI
Fang Wang, Jean Damascene Harindintwali, Zhizhang Yuan

et al.

The Innovation, Journal Year: 2021, Volume and Issue: 2(4), P. 100180 - 100180

Published: Oct. 30, 2021

Language: Английский

Citations

978
Advances and Challenges for the Electrochemical Reduction of CO2 to CO: From Fundamentals to Industrialization DOI
Song Jin,

Zhimeng Hao,

Kai Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(38), P. 20627 - 20648

Published: April 17, 2021

Abstract The electrochemical carbon dioxide reduction reaction (CO 2 RR) provides an attractive approach to convert renewable electricity into fuels and feedstocks in the form of chemical bonds. Among different CO RR pathways, conversion is considered one most promising candidate reactions because its high technological economic feasibility. Integrating catalyst electrolyte design with understanding catalytic mechanism will yield scientific insights promote this technology towards industrial implementation. Herein, we give overview recent advances challenges for selective CO. Multidimensional engineering are also summarized. Furthermore, studies on large‐scale production highlighted facilitate industrialization . To conclude, remaining future directions application generate highlighted.

Language: Английский

Citations

674
Photocatalytic CO2 Reduction to C2+ Products DOI
Josep Albero, Yong Peng, Hermenegildo Garcı́a

et al.

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(10), P. 5734 - 5749

Published: April 17, 2020

There is a considerable interest in the development of photocatalytic CO2 conversion by sunlight, since this process has similarities with natural photosynthesis on which life Earth based. At moment, most efforts field have been aimed at increasing productivity, rather than control product distribution. Particularly, compounds two or more carbons (C2+) higher added value methane, carbon monoxide, formate, are typically major products reduction. This review focuses those reports that described formation atoms reduction either H2O as H2 source electrons and protons. The existing literature organized according to main factor considered be responsible for selectivity C2+ products, including photocatalyst structuration, nature co-catalyst, influence defects, effects surface plasmon band. Emphasis made remarking current empirical knowledge based experimental results lack predictive capability could lead efficient systems production.

Language: Английский

Citations

660
Protecting Copper Oxidation State via Intermediate Confinement for Selective CO2 Electroreduction to C2+ Fuels DOI
Peng‐Peng Yang, Xiaolong Zhang, Fei‐Yue Gao

et al.

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(13), P. 6400 - 6408

Published: March 16, 2020

Selective and efficient catalytic conversion of carbon dioxide (CO2) into value-added fuels feedstocks provides an ideal avenue to high-density renewable energy storage. An impediment enabling deep CO2 reduction oxygenates hydrocarbons (e.g., C2+ compounds) is the difficulty coupling carbon-carbon bonds efficiently. Copper in +1 oxidation state has been thought be active for catalyzing formation, whereas it prone being reduced Cu0 at cathodic potentials. Here we report that catalysts with nanocavities can confine intermediates formed situ, which turn covers local catalyst surface thereby stabilizes Cu+ species. Experimental measurements on multihollow cuprous oxide exhibit a Faradaic efficiency 75.2 ± 2.7% partial current density 267 13 mA cm-2 large C2+-to-C1 ratio ∼7.2. Operando Raman spectra, conjunction X-ray absorption studies, confirm species as-designed are well retained during reduction, leads marked selectivity rate.

Language: Английский

Citations

553
Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO2 Reduction to Formate DOI

Na Han,

Ding Pan, Le He

et al.

Advanced Energy Materials, Journal Year: 2019, Volume and Issue: 10(11)

Published: Dec. 13, 2019

Abstract Selective CO 2 reduction to formic acid or formate is the most technologically and economically viable approach realize electrochemical valorization. Main group metal–based (Sn, Bi, In, Pb, Sb) nanostructured materials hold great promise, but are still confronted with several challenges. Here, current status, challenges, future opportunities of main for reviewed. Firstly, fundamentals presented, including technoeconomic viability different products, possible reaction pathways, standard experimental procedure, performance figures merit. This then followed by detailed discussions about types electrocatalyst materials, an emphasis on underlying material design principles promoting activity, selectivity, stability. Subsequently, recent efforts flow cells membrane electrode assembly reviewed so as promote density well mechanistic studies using in situ characterization techniques. To conclude a short perspective offered directions this exciting field.

Language: Английский

Citations

516
Heterogeneous Single‐Atom Catalysts for Electrochemical CO2 Reduction Reaction DOI
Minhan Li, Haifeng Wang, Wei Luo

et al.

Advanced Materials, Journal Year: 2020, Volume and Issue: 32(34)

Published: July 9, 2020

The electrochemical CO2 reduction reaction (CO2 RR) is of great importance to tackle the rising concentration in atmosphere. RR can be driven by renewable energy sources, producing precious chemicals and fuels, with implementation this process largely relying on development low-cost efficient electrocatalysts. Recently, a range heterogeneous potentially single-atom catalysts (SACs) containing non-precious metals coordinated earth-abundant elements have emerged as promising candidates for RR. Unfortunately, real catalytically active centers key factors that govern catalytic performance these SACs remain ambiguous. Here, ambiguity addressed developing fundamental understanding RR-to-CO SACs, CO accounts major product from SACs. mechanism, rate-determining steps, control activity selectivity are analyzed both experimental theoretical studies. Then, synthesis, characterization, discussed. Finally, challenges future pathways highlighted hope guiding design promote understand

Language: Английский

Citations

491
Metal-free photocatalysts for hydrogen evolution DOI
Mohammad Ziaur Rahman, Md Golam Kibria, C. Buddie Mullins

et al.

Chemical Society Reviews, Journal Year: 2020, Volume and Issue: 49(6), P. 1887 - 1931

Published: Jan. 1, 2020

This article provides a comprehensive review of the latest progress, challenges and recommended future research related to metal-free photocatalysts for hydrogen productionviawater-splitting.

Language: Английский

Citations

456
Insights into the carbon balance for CO2 electroreduction on Cu using gas diffusion electrode reactor designs DOI
Ming Ma, Ezra L. Clark, Kasper T. Therkildsen

et al.

Energy & Environmental Science, Journal Year: 2020, Volume and Issue: 13(3), P. 977 - 985

Published: Jan. 1, 2020

The carbon balance during high-rate CO2 reduction in flow electrolyzers was rigorously analyzed, showing that consumption should be taken into account for evaluating catalytic selectivity of gas products.

Language: Английский

Citations

403
Emerging Dual‐Atomic‐Site Catalysts for Efficient Energy Catalysis DOI
Weiyu Zhang, Yuguang Chao, Wenshu Zhang

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(36)

Published: July 23, 2021

Atomically dispersed metal catalysts with well-defined structures have been the research hotspot in heterogeneous catalysis because of their high atomic utilization efficiency, outstanding activity, and selectivity. Dual-atomic-site (DASCs), as an extension single-atom (SACs), recently drawn surging attention. The DASCs possess higher loading, more sophisticated flexible active sites, offering chance for achieving better catalytic performance, compared SACs. In this review, recent advances on how to design new enhancing energy will be highlighted. It start classification marriage two kinds homonuclear heteronuclear according configuration sites. Then, state-of-the-art characterization techniques discussed. Different synthetic methods applications various reactions, including oxygen reduction reaction, carbon dioxide monoxide oxidation others followed. Finally, major challenges perspectives provided.

Language: Английский

Citations

389
Gas diffusion electrodes (GDEs) for electrochemical reduction of carbon dioxide, carbon monoxide, and dinitrogen to value-added products: a review DOI
Hesamoddin Rabiee, Lei Ge, Xueqin Zhang

et al.

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(4), P. 1959 - 2008

Published: Jan. 1, 2021

Opportunities, challenges and design criteria associated with Gas diffusion electrodes (GDEs) for various electrochemical applications.

Language: Английский

Citations

368