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

Thermal, electrochemical and radiolytic stabilities of ionic liquids DOI
Zhimin Xue, Qin Li, Jingyun Jiang

et al.

Physical Chemistry Chemical Physics, Journal Year: 2018, Volume and Issue: 20(13), P. 8382 - 8402

Published: Jan. 1, 2018

Ionic liquids show instability when exposed to high temperature, voltage as electrolytes, or under irradiation.

Language: Английский

Citations

301
Electrolysis of CO2 to Syngas in Bipolar Membrane-Based Electrochemical Cells DOI
Yuguang Li, Dekai Zhou, Zhifei Yan

et al.

ACS Energy Letters, Journal Year: 2016, Volume and Issue: 1(6), P. 1149 - 1153

Published: Nov. 8, 2016

The electrolysis of CO2 to syngas (CO + H2) using nonprecious metal electrocatalysts was studied in bipolar membrane-based electrochemical cells. Electrolysis carried out aqueous bicarbonate and humidified gaseous on the cathode side cell, with Ag or Bi/ionic liquid electrocatalysts. In both cases, stable currents were observed over a period hours an alkaline electrolyte NiFeOx electrocatalyst anode cell. contrast, performance cells degraded rapidly when conventional anion- cation-exchange membranes used place membrane. agreement earlier reports, Faradaic efficiency for reduction CO high at low overpotential. liquid-phase membrane about 50% 30 mA/cm2 current density. gas-phase densities up 200 could be obtained, albeit lower production. At overpotentials production initially but dropped within 1 h, most likely because dewetting ionic from Bi catalyst surface. effective management protons enables operation possibility practical densities.

Language: Английский

Citations

274
Electrolytic cell design for electrochemical CO2 reduction DOI

Shuyu Liang,

Naveed Altaf, Liang Huang

et al.

Journal of CO2 Utilization, Journal Year: 2019, Volume and Issue: 35, P. 90 - 105

Published: Sept. 24, 2019

Language: Английский

Citations

270
Molybdenum–Bismuth Bimetallic Chalcogenide Nanosheets for Highly Efficient Electrocatalytic Reduction of Carbon Dioxide to Methanol DOI
Xiaofu Sun, Qinggong Zhu, Xinchen Kang

et al.

Angewandte Chemie International Edition, Journal Year: 2016, Volume and Issue: 55(23), P. 6771 - 6775

Published: April 21, 2016

Abstract Methanol is a very useful platform molecule and liquid fuel. Electrocatalytic reduction of CO 2 to methanol promising route, which currently suffers from low efficiency poor selectivity. Herein we report the first work use Mo‐Bi bimetallic chalcogenide (BMC) as an electrocatalyst for reduction. By using BMC on carbon paper electrode 1‐butyl‐3‐methylimidazolium tetrafluoroborate in MeCN electrolyte, Faradaic could reach 71.2 % with current density 12.1 mA cm −2 , much higher than best result reported date. The superior performance resulted excellent synergistic effect Mo Bi producing methanol. reaction mechanism was proposed reason discussed basis some control experiments. This opens way produce efficiently by electrochemical .

Language: Английский

Citations

247
Conversion of CO2to value-added products mediated by ionic liquids DOI
Yu Chen, Tiancheng Mu

Green Chemistry, Journal Year: 2019, Volume and Issue: 21(10), P. 2544 - 2574

Published: Jan. 1, 2019

The thermal, electrochemical and photochemical conversion of CO2mediated by ionic liquids is systematically reviewed.

Language: Английский

Citations

241
CO2reduction: the quest for electrocatalytic materials DOI
Bahareh Khezri,

Adrian C. Fisher,

Martin Pumera

et al.

Journal of Materials Chemistry A, Journal Year: 2017, Volume and Issue: 5(18), P. 8230 - 8246

Published: Jan. 1, 2017

Electrochemical conversion of CO2has attracted attention worldwide since this process can convert carbon dioxide to a wide range value-added chemicals. This reaction required the development efficient electrocatalysts and fundamental understanding kinetics thermodynamics overcome current challenges.

Language: Английский

Citations

240
Cu/Bi metal-organic framework-based systems for an enhanced electrochemical transformation of CO2 to alcohols DOI
Jonathan Albo, Maite Perfecto-Irigaray, Garikoitz Beobide

et al.

Journal of CO2 Utilization, Journal Year: 2019, Volume and Issue: 33, P. 157 - 165

Published: May 25, 2019

Language: Английский

Citations

222
Electrochemical C–N coupling with perovskite hybrids toward efficient urea synthesis DOI Creative Commons
Menglei Yuan, Junwu Chen,

Yiling Bai

et al.

Chemical Science, Journal Year: 2021, Volume and Issue: 12(17), P. 6048 - 6058

Published: Jan. 1, 2021

Electrocatalytic C-N coupling reaction by co-activation of both N2 and CO2 molecules under ambient conditions to synthesize valuable urea opens a new avenue for sustainable development, while the actual catalytic activity is limited poor adsorption capability gas on catalyst surface. Herein, theoretical calculation predicts that well-developed built-in electric field in perovskite hetero-structured BiFeO3/BiVO4 hybrids can accelerate local charge redistribution thus promote targeted activation inert generated electrophilic nucleophilic regions. Thus, heterojunction designed synthesized, which delivers yield rate 4.94 mmol h-1 g-1 with faradaic efficiency 17.18% at -0.4 V vs. RHE 0.1 M KHCO3, outperforming highest values reported as far. The comprehensive analysis further confirms effectively suppresses CO poisoning formation endothermic *NNH intermediate, guarantees exothermic *N[double bond, length m-dash]N* intermediates via reactions form precursor *NCON* intermediate. This work effective electrocatalytic conditions.

Language: Английский

Citations

221
Electrolyte Effects on the Electrochemical Reduction of CO2 DOI Creative Commons
Marília Moura de Salles Pupo, Ruud Kortlever

ChemPhysChem, Journal Year: 2019, Volume and Issue: 20(22), P. 2926 - 2935

Published: Oct. 10, 2019

Abstract The electrochemical reduction of CO 2 to fuels or commodity chemicals is a reaction high interest for closing the anthropogenic carbon cycle. role electrolyte particular interest, as interplay between electrocatalytic surface and plays an important in determining outcome reaction. Therefore, insights on effects are pivotal designing devices that able efficiently selectively convert into valuable products. Here, we provide overview recently obtained discuss how these can be used design parameters construction new systems.

Language: Английский

Citations

212
Enhanced Reduction of CO2 to CO over Cu–In Electrocatalysts: Catalyst Evolution Is the Key DOI Creative Commons
Gastón O. Larrazábal, Antonio J. Martín, Sharon Mitchell

et al.

ACS Catalysis, Journal Year: 2016, Volume and Issue: 6(9), P. 6265 - 6274

Published: Aug. 11, 2016

Copper–indium catalysts have recently shown promising performance for the selective electrochemical reduction of CO2 to CO. In this work, we prepared Cu–In nanoalloys by in situ CuInO2 and In2O3-supported Cu nanoparticles found that structure these evolves substantially over several electrocatalytic cycles, parallel with an increase activity selectivity CO evolution. By combining measurements ex characterization techniques, such as XRD, STEM, elemental mapping, XPS, show behavior is caused segregation copper indium materials, resulting formation a heterogeneous nanostructure Cu-rich cores embedded within In(OH)3 shell-like matrix. The evolved high at moderate overpotential (i.e., jCO > 1.5 mA cm–2 −0.6 V vs RHE). We removal from nanostructures decreases catalysts, particularly terms toward CO, which then recovers reappearance hydroxide following re-equilibration material. On other hand, In(OH)3-supported catalyst exhibits current efficiency comparable without need equilibration stage, indicating plays crucial role favoring production electrocatalysts. These findings shed light on link between architecture materials their underscore potential nonreducible hydroxides act promoters electrocatalysis.

Language: Английский

Citations

188