Unraveling the rate-limiting step of two-electron transfer electrochemical reduction of carbon dioxide DOI Creative Commons
Wanyu Deng, Peng Zhang, Brian Seger

и другие.

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Фев. 10, 2022

Electrochemical reduction of CO2 (CO2ER) has received significant attention due to its potential sustainably produce valuable fuels and chemicals. However, the reaction mechanism is still not well understood. One vital debate whether rate-limiting step (RLS) dominated by availability protons, conversion water molecules, or adsorption CO2. This paper describes insights into RLS investigating pH dependency kinetic isotope effect with respect rate expression CO2ER. Focusing on electrocatalysts geared towards two-electron transfer reactions, we find generation rates CO formate be invariant either deuteration electrolyte over Au, Ag, Sn, In. We elucidate CO2ER onto surface electrocatalysts. expect this finding provide guidance for improving activity through enhancement processes strategies such as modification catalysts careful control pressure interfacial electric field within reactors.

Язык: Английский

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

Zhimeng Hao,

Kai Zhang

и другие.

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(38), С. 20627 - 20648

Опубликована: Апрель 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.

Язык: Английский

Процитировано

684

Active Site Engineering in Porous Electrocatalysts DOI
Hui Chen, Xiao Liang, Yipu Liu

и другие.

Advanced Materials, Год журнала: 2020, Номер 32(44)

Опубликована: Июль 14, 2020

Abstract Electrocatalysis is at the center of many sustainable energy conversion technologies that are being developed to reduce dependence on fossil fuels. The past decade has witnessed significant progresses in exploitation advanced electrocatalysts for diverse electrochemical reactions involved electrolyzers and fuel cells, such as hydrogen evolution reaction (HER), oxygen reduction (ORR), CO 2 (CO RR), nitrogen (NRR), (OER). Herein, recent research advances made porous these five important reviewed. In discussions, an attempt highlight advantages multiobjective optimization surface active sites including not only their density accessibility but also intrinsic activity. First, current knowledge about electrocatalytic briefly summarized. Then, mechanisms above‐mentioned (HER, ORR, RR, NRR, OER), challenges faced by reactions, efforts meet using examined. Finally, future directions synthetic strategies leading materials, insights into sites, standardized tests performance requirements discussed.

Язык: Английский

Процитировано

473

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

и другие.

Energy & Environmental Science, Год журнала: 2021, Номер 14(4), С. 1959 - 2008

Опубликована: Янв. 1, 2021

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

Язык: Английский

Процитировано

376

Discovery of main group single Sb–N4 active sites for CO2 electroreduction to formate with high efficiency DOI

Zhuoli Jiang,

Tao Wang, Jiajing Pei

и другие.

Energy & Environmental Science, Год журнала: 2020, Номер 13(9), С. 2856 - 2863

Опубликована: Янв. 1, 2020

We discover that an Sb single atom material consisting of Sb–N4 moieties anchored on N-doped carbon nanosheets can serve as a CO2RR catalyst to produce formate with high efficiency.

Язык: Английский

Процитировано

314

MOF-based materials for photo- and electrocatalytic CO2 reduction DOI
Xiaofang Li, Qi‐Long Zhu

EnergyChem, Год журнала: 2020, Номер 2(3), С. 100033 - 100033

Опубликована: Май 16, 2020

Язык: Английский

Процитировано

308

Design of a Single‐Atom Indiumδ+–N4Interface for Efficient Electroreduction of CO2to Formate DOI
Huishan Shang, Tao Wang, Jiajing Pei

и другие.

Angewandte Chemie International Edition, Год журнала: 2020, Номер 59(50), С. 22465 - 22469

Опубликована: Сен. 2, 2020

Abstract Main‐group element indium (In) is a promising electrocatalyst which triggers CO 2 reduction to formate, while the high overpotential and low Faradaic efficiency (FE) hinder its practical application. Herein, we rationally design new In single‐atom catalyst containing exclusive isolated δ+ –N 4 atomic interface sites for electroreduction formate with efficiency. This exhibits an extremely large turnover frequency (TOF) up 12500 h −1 at −0.95 V versus reversible hydrogen electrode (RHE), FE of 96 % current density 8.87 mA cm −2 potential −0.65 RHE. Our findings present feasible strategy accurate regulation main‐group catalysts scale.

Язык: Английский

Процитировано

306

Designing a Built-In Electric Field for Efficient Energy Electrocatalysis DOI
Xin Zhao, Mengjie Liu, Yuchao Wang

и другие.

ACS Nano, Год журнала: 2022, Номер 16(12), С. 19959 - 19979

Опубликована: Дек. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Язык: Английский

Процитировано

225

Residual Chlorine Induced Cationic Active Species on a Porous Copper Electrocatalyst for Highly Stable Electrochemical CO2 Reduction to C2+ DOI
Minhan Li, Yuanyuan Ma, Jun Chen

и другие.

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(20), С. 11487 - 11493

Опубликована: Март 8, 2021

Abstract Electrochemical carbon dioxide (CO 2 ) reduction reaction RR) is an attractive approach to deal with the emission of CO and produce valuable fuels chemicals in a carbon‐neutral way. Many efforts have been devoted boost activity selectivity high‐value multicarbon products (C 2+ on Cu‐based electrocatalysts. However, RR electrocatalysts suffer from poor catalytic stability mainly due structural degradation loss active species under condition. To date, most reported present stabilities over dozens hours, which limits advance for RR. Herein, porous chlorine‐doped Cu electrocatalyst exhibits high C Faradaic efficiency (FE) 53.8 % at −1.00 V versus reversible hydrogen electrode (V RHE ). Importantly, catalyst exhibited outstanding long‐term electrocatalysis 240 h. Experimental results show that chlorine‐induced stable cationic 0 /Cu + well‐preserved structure abundant sites are critical FE run electrochemical reduction.

Язык: Английский

Процитировано

209

Heterogeneous catalysts for CO2hydrogenation to formic acid/formate: from nanoscale to single atom DOI
Ruiyan Sun, Yuhe Liao,

Shao‐Tao Bai

и другие.

Energy & Environmental Science, Год журнала: 2021, Номер 14(3), С. 1247 - 1285

Опубликована: Янв. 1, 2021

This review provides an overview of advances on constructing heterogeneous nanostructured and single atom catalysts for CO2hydrogenation to formic acid/formate. The main focus is placed structure–activity correlations mechanistic insights.

Язык: Английский

Процитировано

201

Design strategies for markedly enhancing energy efficiency in the electrocatalytic CO2 reduction reaction DOI
Wenchuan Lai, Yan Qiao, Jiawei Zhang

и другие.

Energy & Environmental Science, Год журнала: 2022, Номер 15(9), С. 3603 - 3629

Опубликована: Янв. 1, 2022

The review summarizes the recent strategies to improve energy efficiency of CO 2 electroreduction, a guiding metric for industrial application and economic feasibility, with emphasis on designing remarkable catalyst advanced electrolysis system.

Язык: Английский

Процитировано

197