Electrocatalyst Microenvironment Engineering for Enhanced Product Selectivity in Carbon Dioxide and Nitrogen Reduction Reactions DOI Creative Commons
Huali Wu, Amrita Singh‐Morgan, Kun Qi

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(8), P. 5375 - 5396

Published: April 6, 2023

Carbon and nitrogen fixation strategies are regarded as alternative routes to produce valuable chemicals used energy carriers fertilizers that traditionally obtained from unsustainable energy-intensive coal gasification (CO CH4), Fischer–Tropsch (C2H4), Haber–Bosch (NH3) processes. Recently, the electrocatalytic CO2 reduction reaction (CO2RR) N2 (NRR) have received tremendous attention, with merits of being both efficient store renewable electricity while providing preparation fossil-fuel-driven reactions. To date, development CO2RR NRR processes is primarily hindered by competitive hydrogen evolution (HER); however, corresponding for inhibiting this undesired side still quite limited. Considering such complex reactions involve three gas–liquid–solid phases successive proton-coupled electron transfers, it appears meaningful review current improving product selectivity in light their respective mechanisms, kinetics, thermodynamics. By examining developments understanding catalyst design, electrolyte engineering, three-phase interface modulation, we discuss key NRR: (i) targeting molecularly defined active sites, (ii) increasing local reactant concentration at (iii) stabilizing confining intermediates.

Language: Английский

Emerging Two-Dimensional Nanomaterials for Electrocatalysis DOI
Huanyu Jin, Chunxian Guo, Xin Liu

et al.

Chemical Reviews, Journal Year: 2018, Volume and Issue: 118(13), P. 6337 - 6408

Published: March 19, 2018

Over the past few decades, design and development of advanced electrocatalysts for efficient energy conversion technologies have been subjects extensive study. With discovery graphene, two-dimensional (2D) nanomaterials emerged as some most promising candidates heterogeneous due to their unique physical, chemical, electronic properties. Here, we review 2D-nanomaterial-based selected electrocatalytic processes. We first discuss advances in 2D based on different compositions functions followed by specific principles. Following this overview, various processes involved water cycle, carbon nitrogen cycle from fundamental conception functional application. place a significant emphasis engineering strategies influence these intrinsic material performance, such properties adsorption energetics. Finally, feature opportunities challenges ahead electrocatalysts. By considering theoretical calculations, surface characterization, electrochemical tests, describe relationships between structure, energy, apparent activity wide variety with goal providing better understanding emerging at atomic level.

Language: Английский

Citations

1822
Fundamentals and Challenges of Electrochemical CO2 Reduction Using Two-Dimensional Materials DOI Creative Commons
Zhenyu Sun, Tao Ma, Hengcong Tao

et al.

Chem, Journal Year: 2017, Volume and Issue: 3(4), P. 560 - 587

Published: Oct. 1, 2017

Language: Английский

Citations

1029
Electrochemical strategies for C–H functionalization and C–N bond formation DOI Creative Commons
Markus D. Kärkäs

Chemical Society Reviews, Journal Year: 2018, Volume and Issue: 47(15), P. 5786 - 5865

Published: Jan. 1, 2018

This review provides an overview of the use electrochemistry as appealing platform for expediting carbon–hydrogen functionalization and carbon–nitrogen bond formation.

Language: Английский

Citations

880
Ionic liquids: a brief history DOI Creative Commons
Tom Welton

Biophysical Reviews, Journal Year: 2018, Volume and Issue: 10(3), P. 691 - 706

Published: April 26, 2018

Abstract There is no doubt that ionic liquids have become a major subject of study for modern chemistry. We used to ever more publications in the field each year, although there some evidence this beginning plateau at approximately 3500 papers year. They been several reviews and books, dealing with different applications aspects their behaviours. In article, I will show little how interest grew developed.

Language: Английский

Citations

827
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
Copper‐Based Metal–Organic Porous Materials for CO2 Electrocatalytic Reduction to Alcohols DOI
Jonathan Albo,

Daniel Vallejo,

Garikoitz Beobide

et al.

ChemSusChem, Journal Year: 2016, Volume and Issue: 10(6), P. 1100 - 1109

Published: Aug. 25, 2016

The electrocatalytic reduction of CO2 has been investigated using four Cu-based metal-organic porous materials supported on gas diffusion electrodes, namely, (1) HKUST-1 framework (MOF), [Cu3 (μ6 -C9 H3 O6 )2 ]n ; (2) CuAdeAce MOF, (μ3 -C5 H4 N5 (3) CuDTA mesoporous aerogel (MOA), [Cu(μ-C2 H2 N2 S2 )]n and (4) CuZnDTA MOA, [Cu0.6 Zn0.4 (μ-C2 . electrodes show relatively high surface areas, accessibilities, exposure the Cu catalytic centers as well favorable performance, that is, they have a efficiency for production methanol ethanol in liquid phase. maximum cumulative Faradaic efficiencies conversion at HKUST-1-, CuAdeAce-, CuDTA-, CuZnDTA-based are 15.9, 1.2, 6, 9.9 %, respectively, current density 10 mA cm-2 , an electrolyte-flow/area ratio 3 mL min gas-flow/area 20 We can correlate these observations with structural features electrodes. Furthermore, HKUST-1- stable performance 17 12 h, respectively.

Language: Английский

Citations

373
Continuous-flow electroreduction of carbon dioxide DOI Creative Commons
Balázs Endrődi, Gábor Bencsik, Ferenç Darvas

et al.

Progress in Energy and Combustion Science, Journal Year: 2017, Volume and Issue: 62, P. 133 - 154

Published: June 13, 2017

Solar fuel generation through electrochemical CO2 conversion offers an attractive avenue to store the energy of sunlight in form chemical bonds, with simultaneous remediation a greenhouse gas. While impressive progress has been achieved developing novel nanostructured catalysts and understanding mechanistic details this process, limited knowledge gathered on continuous-flow reactors for electroreduction. This is indeed surprising considering that might be only way scale-up fledgling technology future industrial application. In review article, we discuss parameters influence performance flow electrolyzers. analysis spans overall design cell (microfluidic or membrane-based), employed materials (catalyst, support, etc.), operational conditions (electrolyte, pressure, temperature, etc.). We highlight R&D avenues offering particularly promising development opportunities together intrinsic limitations different approaches. By collecting most relevant characterization methods (together descriptive parameters), also present assessment framework benchmarking Finally, give brief outlook photoelectrochemical where solar input directly utilized.

Language: Английский

Citations

346
A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction DOI Creative Commons
Jiaqi Feng, Hongshuai Gao, Lirong Zheng

et al.

Nature Communications, Journal Year: 2020, Volume and Issue: 11(1)

Published: Aug. 28, 2020

Abstract Developing effective catalysts based on earth abundant elements is critical for CO 2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and current density of ( j ) remains challenge. Herein, we prepare Mn single-atom catalyst (SAC) with Mn-N 3 site embedded in graphitic carbon nitride. The prepared exhibits 98.8% FE 14.0 mA cm −2 at low overpotential 0.44 V aqueous electrolyte, outperforming all reported SACs. Moreover, higher 29.7 obtained an ionic liquid electrolyte 0.62 overpotential. In situ X-ray absorption spectra functional theory calculations demonstrate that the remarkable performance attributed to site, which facilitates formation key intermediate COOH * through lowered free energy barrier.

Language: Английский

Citations

346
Solvents and Supporting Electrolytes in the Electrocatalytic Reduction of CO2 DOI Creative Commons
Maximilian König, Jan Vaes, Elias Klemm

et al.

iScience, Journal Year: 2019, Volume and Issue: 19, P. 135 - 160

Published: July 16, 2019

Different electrolytes applied in the aqueous electrocatalytic CO2 reduction reaction (CO2RR) considerably influence catalyst performance. Their concentration, species, buffer capacity, and pH value local conditions impact product distribution of electrocatalyst. Relevant properties prospective solvents include their basicity, solubility, conductivity, toxicity, which affect CO2RR applicability solvents. The complexity an electrochemical system impedes direct correlation between a single parameter cell performance indicators such as Faradaic efficiency; thus effects different are often not fully comprehended. For industrial application, deeper understanding described this review can help with prediction performance, well development scalable electrolyzers. In review, application supporting reported literature summarized discussed.

Language: Английский

Citations

333
Unveiling Electrochemical Urea Synthesis by Co‐Activation of CO2 and N2 with Mott–Schottky Heterostructure Catalysts DOI
Menglei Yuan, Junwu Chen,

Yiling Bai

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(19), P. 10910 - 10918

Published: Feb. 26, 2021

Abstract Electrocatalytic C−N bond coupling to convert CO 2 and N molecules into urea under ambient conditions is a promising alternative harsh industrial processes. However, the adsorption activation of inert gas then driving C–N reaction energetically challenging. Herein, novel Mott–Schottky Bi‐BiVO 4 heterostructures are described that realize remarkable yield rate 5.91 mmol h −1 g Faradaic efficiency 12.55 % at −0.4 V vs. RHE. Comprehensive analysis confirms emerging space–charge region in heterostructure interface not only facilitates targeted on generated local nucleophilic electrophilic regions, but also effectively suppresses poisoning formation endothermic *NNH intermediates. This guarantees desired exothermic *N=N* intermediates form precursor, *NCON*.

Language: Английский

Citations

309