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

Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte DOI Creative Commons
Stephanie Nitopi, Erlend Bertheussen, Søren B. Scott

et al.

Chemical Reviews, Journal Year: 2019, Volume and Issue: 119(12), P. 7610 - 7672

Published: May 22, 2019

To date, copper is the only heterogeneous catalyst that has shown a propensity to produce valuable hydrocarbons and alcohols, such as ethylene ethanol, from electrochemical CO2 reduction (CO2R). There are variety of factors impact CO2R activity selectivity, including surface structure, morphology, composition, choice electrolyte ions pH, cell design. Many these often intertwined, which can complicate discovery design efforts. Here we take broad historical view different aspects their complex interplay in catalysis on Cu, with purpose providing new insights, critical evaluations, guidance field regard research directions best practices. First, describe various experimental probes complementary theoretical methods have been used discern mechanisms by products formed, next present our current understanding reaction networks for Cu. We then analyze two key attempts alter selectivity Cu: nanostructuring formation bimetallic electrodes. Finally, offer some perspectives future outlook CO2R.

Language: Английский

Citations

3698
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels DOI
Yuvraj Y. Birdja, Elena Pérez‐Gallent, Marta C. Figueiredo

et al.

Nature Energy, Journal Year: 2019, Volume and Issue: 4(9), P. 732 - 745

Published: Sept. 9, 2019

Language: Английский

Citations

2101
Electrocatalysis for CO2conversion: from fundamentals to value-added products DOI

Genxiang Wang,

Junxiang Chen, Yichun Ding

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(8), P. 4993 - 5061

Published: Jan. 1, 2021

This timely and comprehensive review mainly summarizes advances in heterogeneous electroreduction of CO2: from fundamentals to value-added products.

Language: Английский

Citations

897
Understanding the Roadmap for Electrochemical Reduction of CO2 to Multi-Carbon Oxygenates and Hydrocarbons on Copper-Based Catalysts DOI
Yao Zheng, Anthony Vasileff, Xianlong Zhou

et al.

Journal of the American Chemical Society, Journal Year: 2019, Volume and Issue: 141(19), P. 7646 - 7659

Published: April 15, 2019

Electrochemical reduction of CO2 to high-energy-density oxygenates and hydrocarbons beyond CO is important for long-term large-scale renewable energy storage. However, the key step C-C bond formation needed generation C2 products induces an additional barrier on reaction. This inevitably creates larger overpotentials greater variety as compared conversion C1 products. Therefore, in-depth understanding catalytic mechanism required advancing design efficient electrocatalysts control reaction pathway desired Herein, we present a critical appraisal focusing connection between fundamentals electrocatalysts. An discussion mechanistic aspects various pathways copper-based catalysts presented together with consideration practical factors under electrocatalytic operating conditions. By providing some typical examples illustrating benefit merging theoretical calculations, surface characterization, electrochemical measurements, try address issues ongoing debate toward better at atomic level envisioning roadmap generation.

Language: Английский

Citations

889
Surface strategies for catalytic CO2reduction: from two-dimensional materials to nanoclusters to single atoms DOI
Liming Wang, Wenlong Chen, Doudou Zhang

et al.

Chemical Society Reviews, Journal Year: 2019, Volume and Issue: 48(21), P. 5310 - 5349

Published: Jan. 1, 2019

This work constructively reviewed and predicted the surface strategies for catalytic CO2reduction with 2D material, nanocluster single-atom catalysts

Language: Английский

Citations

748
Surface and Interface Control in Nanoparticle Catalysis DOI
Chenlu Xie, Zhiqiang Niu, Dohyung Kim

et al.

Chemical Reviews, Journal Year: 2019, Volume and Issue: 120(2), P. 1184 - 1249

Published: Oct. 3, 2019

The surface and interfaces of heterogeneous catalysts are essential to their performance as they often considered be active sites for catalytic reactions. With the development nanoscience, ability tune interface nanostructures has provided a versatile tool optimization catalyst. In this Review, we present control nanoparticle in context oxygen reduction reaction (ORR), electrochemical CO2 (CO2 RR), tandem catalysis three sections. first section, start with activity ORR on nanoscale then focus approaches optimize Pt-based catalyst including using alloying, core-shell structure, high area open structures. section RR, where composition plays dominant role, cover its fundamentals different nanosized metal catalysts. For catalysis, adjacent single nanostructure catalyze sequential reactions, describe concept principle, synthesis methodology, application

Language: Английский

Citations

666
Core–shell structured catalysts for thermocatalytic, photocatalytic, and electrocatalytic conversion of CO2 DOI Creative Commons
Sonali Das, Javier Pérez‐Ramírez, Jinlong Gong

et al.

Chemical Society Reviews, Journal Year: 2020, Volume and Issue: 49(10), P. 2937 - 3004

Published: Jan. 1, 2020

Catalytic conversion of CO2 to produce fuels and chemicals is attractive in prospect because it provides an alternative fossil feedstocks the benefit converting cycling greenhouse gas on a large scale. In today's technology, converted into hydrocarbon Fischer-Tropsch synthesis via water shift reaction, but processes for direct such as methane, methanol, C2+ hydrocarbons or syngas are still far from large-scale applications processing challenges that may be best addressed by discovery improved catalysts-those with enhanced activity, selectivity, stability. Core-shell structured catalysts relatively new class nanomaterials allow controlled integration functions complementary materials optimised compositions morphologies. For conversion, core-shell can provide distinctive advantages addressing catalyst sintering activity loss reforming processes, insufficient product selectivity thermocatalytic hydrogenation, low efficiency photocatalytic electrocatalytic hydrogenation. preceding decade, substantial progress has been made synthesis, characterization, evaluation potential applications. Nonetheless, remain inexpensive, robust, regenerable this class. This review in-depth assessment these thermocatalytic, photocatalytic, valuable hydrocarbons.

Language: Английский

Citations

657
pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper DOI Creative Commons
Xinyan Liu, Philomena Schlexer, Jianping Xiao

et al.

Nature Communications, Journal Year: 2018, Volume and Issue: 10(1)

Published: Dec. 28, 2018

Abstract We present a microkinetic model for CO (2) reduction (CO R) on Cu(211) towards C 2 products, based energetics estimated from an explicit solvent model. show that the differences in both Tafel slopes and pH dependence 1 vs activity arise their multi-step mechanisms. find depletion products observed at high overpotential to nd order of C-C coupling coverage, which decreases due competition pathway. further demonstrate fixed yield similar activities, facile kinetics Cu, suggests be favored R under alkaline conditions. The mechanistic insights this work elucidate how reaction conditions can lead significant enhancements selectivity higher value products.

Language: Английский

Citations

534
High-rate electroreduction of carbon monoxide to multi-carbon products DOI
Matthew Jouny, Wesley Luc, Feng Jiao

et al.

Nature Catalysis, Journal Year: 2018, Volume and Issue: 1(10), P. 748 - 755

Published: Aug. 17, 2018

Language: Английский

Citations

525
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