Tuning the CO2 and CO Electroreduction by Rate-Determining and Selectivity-Determining Steps DOI

Yuanyuan Xue,

Lijuan Zhang,

Min Kuang

et al.

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 16, 2025

The renewable electricity-driven CO2 and CO reduction represents a promising approach for reducing the footprint toward carbon neutrality. Substantial research developments have been achieved in designing catalysts reaction interfaces enhanced electrocatalytic activity selectivity, investigation understanding of complex mechanisms also extensively investigated by both situ characterizations theoretical investigations. Although quasi-equilibrium rate-determining step assumptions are widely used electrochemical kinetics, overall rate is generally determined series elementary steps, influence certain can be quantified based on degree control theory. For complicated networks CO(2) reduction, not only steps but subsequent selectivity-determining play critical roles, especially product selectivity. In this Perspective, we summarize strategies that tune selectivity their impacts respectively. addition, describe coupling electroreduction with other (electro)chemical reactions, such as nitrite methane oxidation, to form value-added products. At end, current challenges opportunities field discussed inspire further development next stage.

Language: Английский

In-situ characterization technologies and theoretical calculations in carbon dioxide reduction: In-depth understanding of reaction mechanisms and rational design of electrocatalysts DOI
Rutao Wang, Xiaokun Yang, Jianpeng Zhang

et al.

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 533, P. 216541 - 216541

Published: Feb. 28, 2025

Language: Английский

Citations

1

Ethylene Electrosynthesis via Selective CO2 Reduction: Fundamental Considerations, Strategies, and Challenges DOI

Thomas O' Carroll,

Xiaoxuan Yang,

Kenneth J. Gordon

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown

Published: June 11, 2024

Abstract The electrochemical carbon dioxide reduction reaction (CO 2 RR) is a promising approach for reducing atmospheric ) emissions, allowing harmful CO to be converted into more valuable carbon‐based products. On one hand, single (C 1 products have been obtained with high efficiency and show great promise industrial capture. However, multi‐carbon 2+ possess market value demonstrated significant as potential RR. Due RR's multiple pathways similar equilibrium potentials, the extended mechanisms necessary form C continue reduce overall selectivity of ‐to‐C electroconversion. Meanwhile, RR whole faces many challenges relating system optimization, owing an intolerance low surface pH, systemic stability utilization issues, competing side in H evolution (HER). Ethylene 4 remains incredibly within chemical industry; however, current established method producing ethylene (steam cracking) contributes emission atmosphere. Thus, strategies significantly increase this technology are essential. This review will discuss vital factors influencing forming summarize recent advancements electrosynthesis.

Language: Английский

Citations

8

Zn-Cu Bimetallic Gas Diffusion Electrodes for Electrochemical Reduction of CO2 to Ethylene DOI
Munzir H. Suliman,

Hussain Al Naji,

Muhammad Usman

et al.

Electrochimica Acta, Journal Year: 2024, Volume and Issue: 500, P. 144723 - 144723

Published: July 25, 2024

Language: Английский

Citations

7

Research Progress of Dual‐Site Tandem Catalysts in the Preparation of Multi Carbon Products by Electro Reduction of CO2 DOI Open Access
Wenjing Xu, Huishan Shang, Jie Guan

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 12, 2024

Abstract The era of an energy economy driven by “carbon neutrality” is putting forward stricter requirements for the use carbon resources and governance CO 2 . Electrochemical reduction dioxide reaction (CO RR), renewable energy, a practical storage technology with broad application prospects. It can reduce into carbon‐based fuels chemical products. Among them, multi‐carbon (C 2+ ) products have higher density larger market size, significantly global demand fossil close artificial cycle. Introducing additional active sites Cu‐based catalysts to prepare dual‐site tandem regulate electronic geometric structure catalysts, break linear scale relationships, potential barriers, bring superb stable catalytic performance. Various types are developed, understanding effect pushed level. This paper reviews several typical catalysts: atom–atom atom‐particle particle–particle heterogeneous interface catalysts. then deeply analyzes mechanism research progress these advanced in RR. In addition, challenges opportunities faced such also discussed.

Language: Английский

Citations

6

Theoretical design of dual-site metallo-covalent organic frameworks for efficient CO2 photoreduction into C2H4 DOI

K.M Chen,

Ya Wang,

Yuqi Dong

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 365, P. 124933 - 124933

Published: Dec. 11, 2024

Language: Английский

Citations

6

In Situ Raman Spectroscopic Studies of Electrochemical CO2 Reduction on Cu-Based Electrodes DOI

Zi‐Yu Du,

Kun Wang,

Si-Bo Li

et al.

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(28), P. 11741 - 11755

Published: July 9, 2024

The electrochemical CO2 reduction reaction (CO2RR), which utilizes renewable energy to produce carbon-neutral chemicals and fuels, offers a potential pathway toward achieving global carbon neutrality. Cu-based catalysts have gained significant attention in this field due their unique coupling ability convert into multicarbon products, while maintaining high Faradaic efficiency. However, the CO2RR process is complex, involving multistep proton–electron transfer that involves intermediates associated with carbon- oxygen-containing species. Therefore, work aims review recent progress of situ surface-enhanced Raman spectroscopic (SERS) studies on catalysts. possible mechanism has been first discussed. In SERS single-crystal electrodes nanocatalysts different electronic states, morphologies, compositions reviewed, various during captured clarify mechanisms structure–activity relationships. Moreover, future opportunities challenges for electrocatalysis are presented. This will provide fundamental insights understanding design more efficient, selective, stable

Language: Английский

Citations

5

Atomic Design of Copper Active Sites in Pristine Metal–Organic Coordination Compounds for Electrocatalytic Carbon Dioxide Reduction DOI Creative Commons
Juan Wang, Qingbo Wa,

Qi Diao

et al.

Small Methods, Journal Year: 2024, Volume and Issue: 8(11)

Published: May 20, 2024

Abstract Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) has emerged as a promising and sustainable approach to cut emissions by converting greenhouse gas CO value‐added chemicals fuels. Metal–organic coordination compounds, especially the copper (Cu)‐based which feature well‐defined crystalline structures designable metal active sites, have attracted much research attention in electrocatalytic RR. Herein, recent advances of electrochemical RR on pristine Cu‐based compounds with different types Cu sites are reviewed. First, general pathways briefly introduced. Then highly efficient conversion various kinds (e.g., single‐Cu site, dimeric‐Cu multi‐Cu heterometallic site) is systematically discussed, along corresponding catalytic mechanisms. Finally, some existing challenges potential opportunities for this direction provided guide rational design metal–organic their practical application

Language: Английский

Citations

4

Constructing an Active Sulfur‐Vacancy‐Rich Surface for Selective *CH3‐CH3 Coupling in CO2‐to‐C2H6 Conversion With 92% Selectivity DOI Open Access

Xiaonan Yang,

Liteng Ren,

Zhiheng Chen

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 6, 2024

Abstract To achieve high selectivity in photocatalytic CO 2 reduction to C 2+ products, increasing the number of adsorption sites and lowering energy barriers for key intermediates are critical. A ZnIn S 4 (ZIS)/MoO 3‐x (Z‐M) photocatalyst is presented, which plasmonic MoO generates hot electrons, creating a multielectron environment ZIS that facilitates efficient C─C coupling reactions. Density functional theory (DFT) calculations reveal reduces formation sulfur vacancies (S V ) ZIS, thereby enhancing activation. The ‐rich surface lowers barrier forming HCOO * −0.33 eV whereas COOH 0.77 eV. Successive hydrogenation leads CH , converts 3 with an −0.63 ‐CH 0.54 eV, lower than 0.73 form H . Thus, Z‐M preferentially produces 6 over Under visible light, achieves ‐to‐C conversion rate 467.3 µmol g −1 h 92.0% selectivity. This work highlights dual role photocatalysts improving production reduction.

Language: Английский

Citations

4

Selective Photocatalytic Conversion of CO2 to Ethanol via Unsaturated Cu–O Domains DOI
Qiang Wang, Mingqi He, Pengxin Yang

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 22, 2024

Enhancing the selectivity of photocatalytic CO2 reduction to valuable multicarbon (C2+) products remains a significant challenge in green synthetic chemistry. Here, we present dual-center strategy for metal oxides that boosts photochemical conversion ethanol by regulating coordination number and oxygen sites. Notably, CuO catalysts rich low-coordinated Cu–O domains have achieved nearly perfect (96.9%), extraordinary durability (60 h), superior yield rate 30.5 μmol·g–1·h–1, surpassing performance many existing photocatalysts water vapor CO2. Density functional theory calculations operando spectroscopic results provide conclusive evidence tricoordinated copper (Cu3c) increases coverage key *CO species, while bicoordinated (O2c) controls migration thereby effectively reducing energy requirement dimerization into *OC–CO intermediates (ΔG*OC–CO = −0.56 eV) pathway. This work offers insights designing exhibit improved C2+ fuels.

Language: Английский

Citations

4

Enhanced CO2 Electroreduction to ethylene on Cu nanocube coated with nitrogen-doped carbon shell in-situ electro-derived from metal-organic framework DOI
Na Zhang, Yunlong Zhang

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 499, P. 156694 - 156694

Published: Oct. 13, 2024

Language: Английский

Citations

4