Computational Methods in Heterogeneous Catalysis DOI
Benjamin W. J. Chen, Lang Xu, Manos Mavrikakis

et al.

Chemical Reviews, Journal Year: 2020, Volume and Issue: 121(2), P. 1007 - 1048

Published: Dec. 22, 2020

The unprecedented ability of computations to probe atomic-level details catalytic systems holds immense promise for the fundamentals-based bottom-up design novel heterogeneous catalysts, which are at heart chemical and energy sectors industry. Here, we critically analyze recent advances in computational catalysis. First, will survey progress electronic structure methods atomistic catalyst models employed, have enabled catalysis community build increasingly intricate, realistic, accurate active sites supported transition-metal catalysts. We then review developments microkinetic modeling, specifically mean-field kinetic Monte Carlo simulations, bridge gap between nanoscale insights macroscale experimental kinetics data with increasing fidelity. finally advancements theoretical accelerating discovery. Throughout review, provide ample examples applications, discuss remaining challenges, our outlook near future.

Language: Английский

Gas-Diffusion Electrodes for Carbon Dioxide Reduction: A New Paradigm DOI
Drew Higgins, Christopher Hahn, Chengxiang Xiang

et al.

ACS Energy Letters, Journal Year: 2018, Volume and Issue: 4(1), P. 317 - 324

Published: Dec. 14, 2018

Significant advances have been made in recent years discovering new electrocatalysts and developing a fundamental understanding of electrochemical CO2 reduction processes. This field has progressed to the point that efforts can now focus on translating this knowledge toward development practical electrolyzers, which potential replace conventional petrochemical processes as sustainable route produce fuels chemicals. In Perspective, we take critical look at progress incorporating catalysts into device architectures operate using vapor-phase reactants, thereby overcoming intrinsic limitations aqueous-based systems. Performance comparison is between state-of-the-art electrolyzers commercial H2O electrolyzers—a well-established technology provides realistic performance targets. Beyond just higher rates, vapor-fed reactors represent paradigms for unprecedented control local reaction conditions, provide perspective challenges opportunities generating achieving technological electrolyzers.

Language: Английский

Citations

514

Photoelectrochemical Conversion of Carbon Dioxide (CO2) into Fuels and Value-Added Products DOI Creative Commons
Vignesh Kumaravel, John Bartlett, Suresh C. Pillai

et al.

ACS Energy Letters, Journal Year: 2020, Volume and Issue: 5(2), P. 486 - 519

Published: Jan. 8, 2020

The conversion of carbon dioxide (CO2) into fuels and value-added products is one the most significant inventions to address global warming energy needs. Photoelectrochemical (PEC) CO2 can be considered as an artificial photosynthesis technique that produces formate, formaldehyde, formic acid, methane, methanol, ethanol, etc. Recent advances in electrode materials, mechanisms, kinetics, thermodynamics, reactor designs PEC have been comprehensively reviewed this article. adsorption activation CO2/intermediates at surface are key steps for improving kinetics conversion. efficiency could upgraded through utilization 2D/3D plasmonic metals, carbon-based catalysts, porous nanostructures, metal–organic frameworks, molecular biological molecules. defect engineered (by cation/anion vacancy, crystal distortion, pits, creation oxygen vacancies) Z-scheme heterojunctions, bioelectrodes, tandem photovoltaic–PEC reactors suitable options enhance low external bias.

Language: Английский

Citations

481

Structural Sensitivities in Bimetallic Catalysts for Electrochemical CO2 Reduction Revealed by Ag–Cu Nanodimers DOI
Jianfeng Huang, Mounir Mensi, Emad Oveisi

et al.

Journal of the American Chemical Society, Journal Year: 2019, Volume and Issue: 141(6), P. 2490 - 2499

Published: Jan. 18, 2019

Understanding the structural and compositional sensitivities of electrochemical CO2 reduction reaction (CO2RR) is fundamentally important for developing highly efficient selective electrocatalysts. Here, we use Ag/Cu nanocrystals to uncover key role played by interface in promoting CO2RR. Nanodimers including two constituent metals as segregated domains sharing a tunable are obtained seeded growth synthesis, wherein preformed Ag nanoparticles used nucleation seeds Cu domain. We find that type metal precursor strength reducing agent play achieving desired chemical control. show tandem catalysis electronic effects, both enabled addition form nanodomain within same catalyst, synergistically account an enhancement Faradaic efficiency C2H4 3.4-fold partial current density 2-fold compared with pure counterpart. The insights gained from this work may be beneficial designing multicomponent catalysts reduction.

Language: Английский

Citations

479

Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment DOI Creative Commons
Zhuo Xing, Lin Hu,

Donald S. Ripatti

et al.

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

Published: Jan. 8, 2021

Electroreduction of carbon dioxide (CO

Language: Английский

Citations

458

Electrocatalytic reduction of CO2 and CO to multi-carbon compounds over Cu-based catalysts DOI
Wenchao Ma, Xiaoyang He, Wei Wang

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(23), P. 12897 - 12914

Published: Jan. 1, 2021

This tutorial review discusses the similarities and differences between electrocatalytic reduction of CO 2 to C 2+ olefins oxygenates over Cu-based catalysts.

Language: Английский

Citations

454

A Highly Porous Copper Electrocatalyst for Carbon Dioxide Reduction DOI
Jingjing Lv, Matthew Jouny, Wesley Luc

et al.

Advanced Materials, Journal Year: 2018, Volume and Issue: 30(49)

Published: Oct. 10, 2018

Abstract Electrochemical reduction of carbon dioxide (CO 2 ) is an appealing approach toward tackling climate change associated with atmospheric CO emissions. This uses as the feedstock to produce value‐added chemicals, resulting in a carbon‐neutral (or even carbon‐negative) process for chemical production. Many efforts have been devoted development electrolysis devices that can be operated at industrially relevant rates; however, limited progress has made, especially valuable C 2+ products. Herein, nanoporous copper catalyst synthesized and integrated into microfluidic flow cell electrolyzer. The electrolyzer exhibits current density 653 mA cm −2 product selectivity ≈62% applied potential −0.67 V (vs reversible hydrogen electrode). highly porous electrode structure facilitates rapid gas transport across electrode–electrolyte interface high densities. Further investigations on electrolyte effects reveal surface pH value substantially different from bulk electrolyte, nonbuffering near‐neutral electrolytes when operating currents.

Language: Английский

Citations

437

Mechanistic Understanding of CO2 Reduction Reaction (CO2RR) Toward Multicarbon Products by Heterogeneous Copper-Based Catalysts DOI
Tanya K. Todorova,

Moritz W. Schreiber,

Marc Fontecave

et al.

ACS Catalysis, Journal Year: 2019, Volume and Issue: 10(3), P. 1754 - 1768

Published: Dec. 30, 2019

In the recent years, significant progress has been made toward designing active and selective catalysts for electrochemical CO2 reduction, with particular interest focused on two major C2 products—ethylene ethanol. Numerous efforts have to enhance understanding of heterogeneous copper-based reduction mechanisms by computational studies. Here we provide a critical assessment various proposed scenarios initial post C–C coupling steps that result in either ethylene or silico rationalization parameters controlling product selectivity, such as catalyst structure composition (Cu facets, presence defective sites and/or subsurface oxygen atoms, interplay second metal) reaction conditions (pH, applied potential, electrolyte), is provided. A comprehensive scheme combining pathways derived, issues are still under debate require further investigations highlighted.

Language: Английский

Citations

431

Advances and challenges in electrochemical CO2reduction processes: an engineering and design perspective looking beyond new catalyst materials DOI Open Access
Sahil Garg, Mengran Li, Adam Z. Weber

et al.

Journal of Materials Chemistry A, Journal Year: 2019, Volume and Issue: 8(4), P. 1511 - 1544

Published: Dec. 12, 2019

This review of design and operating conditions electrochemical CO2reduction covers electrolytes, electrodes, reactors, temperature, pressure, pH effects.

Language: Английский

Citations

382

Electrochemical CO2 reduction (CO2RR) to multi-carbon products over copper-based catalysts DOI Creative Commons
Abebe Reda Woldu, Zanling Huang, Pengxiang Zhao

et al.

Coordination Chemistry Reviews, Journal Year: 2021, Volume and Issue: 454, P. 214340 - 214340

Published: Dec. 13, 2021

Language: Английский

Citations

371

Carbon monoxide electroreduction as an emerging platform for carbon utilization DOI
Matthew Jouny, Gregory S. Hutchings, Feng Jiao

et al.

Nature Catalysis, Journal Year: 2019, Volume and Issue: 2(12), P. 1062 - 1070

Published: Dec. 9, 2019

Language: Английский

Citations

364