Pd-Decorated Cu2O–Ag Catalyst Promoting CO2 Electroreduction to C2H4 by Optimizing CO Intermediate Adsorption and Hydrogenation DOI
Xianbin Xu,

Difei Xiao,

Yugang Gao

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(13), P. 16243 - 16252

Published: March 25, 2024

Electrocatalytic CO2 reduction reaction (CO2RR) to high value-added products, such as ethylene (C2H4), offers a promising approach achieve carbon neutrality. Although recent studies have reported that tandem catalyst (for example, Cu–Ag systems) exhibits advantage in C2H4 production, its practical application is largely inhibited by the following: (1) traditional cannot effectively stabilize *CO intermediate, resulting sluggish C–C coupling, and (2) inadequate H2O activation ability hinders hydrogenation of intermediates. To break through above bottleneck, herein, palladium (Pd) was introduced into Cu2O–Ag, typical conventional catalyst, construct Cu2O–Pd–Ag ternary catalyst. Extensive experiment density functional theory calculation prove Pd can efficiently intermediate promote activation, which contributes coupling hydrogenation, key steps conversion C2H4. Beneficial efficient synergy Cu2O, Pd, Ag, optimal achieves CO2RR toward with faradaic efficiency 63.2% at −1.2 VRHE, higher than achieved Cu2O–Ag most other catalysts. This work fruitful exploration rare providing new route for constructing an electrocatalyst.

Language: Английский

Electrochemical reduction of carbon dioxide to multicarbon (C2+) products: challenges and perspectives DOI Creative Commons
Bin Chang, Hong Pang,

Fazal Raziq

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(11), P. 4714 - 4758

Published: Jan. 1, 2023

This review analyzes advanced catalysts and C 2+ synthesis mechanisms based on theoretical explorations in situ / operando characterizations. Triphasic interface optimization is discussed for the potential of industry-compatible stability.

Language: Английский

Citations

197
Multiscale CO2 Electrocatalysis to C2+ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication DOI
Tianxiang Yan, Xiaoyi Chen,

Lata Kumari

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(17), P. 10530 - 10583

Published: Aug. 17, 2023

Electrosynthesis of value-added chemicals, directly from CO2, could foster achievement carbon neutral through an alternative electrical approach to the energy-intensive thermochemical industry for utilization. Progress in this area, based on electrogeneration multicarbon products CO2 electroreduction, however, lags far behind that C1 products. Reaction routes are complicated and kinetics slow with scale up high levels required commercialization, posing significant problems. In review, we identify summarize state-of-art progress synthesis a multiscale perspective discuss current hurdles be resolved generation reduction including atomistic mechanisms, nanoscale electrocatalysts, microscale electrodes, macroscale electrolyzers guidelines future research. The review ends cross-scale links discrepancies between different approaches extensions performance stability issues arise industrial environment.

Language: Английский

Citations

143
Hydrophobic, Ultrastable Cuδ+ for Robust CO2 Electroreduction to C2 Products at Ampere-Current Levels DOI

Mingwei Fang,

Meiling Wang, Zewen Wang

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(20), P. 11323 - 11332

Published: May 11, 2023

Copper (Cu) is the only known material that can efficiently electrocatalyze CO2 to value-added multicarbon products. Owing instability of Cuδ+ state and microscopic structure in reactions, Cu catalysts are still facing big challenges with low selectivity poor durability, particularly at high current densities. Herein, we report a rational one-step surface coordination approach for synthesis dendrites an ultrastable hydrophobicity (Cu CF), even after exposure air over 6 months. As result, CF exhibited C2 FE 90.6% partial density 453.3 mA cm-2 flow cell. A 400 h stable electrolysis 800 ground-breaking operation large industrial 10 were achieved membrane electrode assembly (MEA) form. We further demonstrated continuous production C2H5OH solution 90% relative purity 600 50 solid-electrolyte reactor. Spectroscopy computation results suggested Cu(II) carboxylate species formed on CF, which ensured stability hydrophobicity. rich active sites three-phase interface catalyst achieved, along optimized *CO adsorption strength configuration. The mixed configurations made dimerization process easier, promoted conversion This work provides promising paradigm design development Cu-based ultrahigh under

Language: Английский

Citations

137
Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering DOI Creative Commons

Junpeng Qu,

Xianjun Cao,

Gao Li

et al.

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: July 11, 2023

Electrochemical carbon dioxide reduction reaction (CO2RR) provides a promising way to convert CO2 chemicals. The multicarbon (C2+) products, especially ethylene, are of great interest due their versatile industrial applications. However, selectively reducing ethylene is still challenging as the additional energy required for C-C coupling step results in large overpotential and many competing products. Nonetheless, mechanistic understanding key steps preferred pathways/conditions, well rational design novel catalysts production have been regarded approaches achieving highly efficient selective CO2RR. In this review, we first illustrate CO2RR (e.g., adsorption/activation, formation *CO intermediate, step), offering conversion ethylene. Then alternative pathways conditions competitive products (C1 other C2+ products) investigated, guiding further development generation. Engineering strategies Cu-based CO2RR-ethylene summarized, correlations mechanism/pathways, engineering selectivity elaborated. Finally, major challenges perspectives research area proposed future practical

Language: Английский

Citations

56
Engineering Cu(I)/Cu(0) interfaces for efficient ethanol production from CO2 electroreduction DOI Creative Commons

Rongming Cai,

Mingzi Sun, Fei Yang

et al.

Chem, Journal Year: 2023, Volume and Issue: 10(1), P. 211 - 233

Published: Sept. 21, 2023

Language: Английский

Citations

53
Zeolitic imidazolate framework-67 and its derivatives for photocatalytic applications DOI

Zhenlu Liu,

Dengrong Sun, Changshui Wang

et al.

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 502, P. 215612 - 215612

Published: Dec. 18, 2023

Language: Английский

Citations

50
Local CO2 reservoir layer promotes rapid and selective electrochemical CO2 reduction DOI Creative Commons
Subhabrata Mukhopadhyay, Muhammad Saad Naeem, G. Shiva Shanker

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: April 22, 2024

Abstract Electrochemical CO 2 reduction reaction in aqueous electrolytes is a promising route to produce added-value chemicals and decrease carbon emissions. However, even Gas-Diffusion Electrode devices, low solubility limits catalysis rate selectivity. Here, we demonstrate that when assembled over heterogeneous electrocatalyst, film of nitrile-modified Metal-Organic Framework (MOF) acts as remarkable -solvation layer increases its local concentration by ~27-fold compared bulk electrolyte, reaching 0.82 M. When mounted on Bi catalyst Gas Diffusion Electrode, the MOF drastically improves -to-HCOOH conversion, above 90% selectivity partial HCOOH currents 166 mA/cm (at −0.9 V vs RHE). The also facilitates through stabilization intermediates, identified operando infrared spectroscopy Density Functional Theory. Hence, presented strategy provides new molecular means enhance electrochemical reaction, leading it closer requirements for practical implementation.

Language: Английский

Citations

37
Recent Progress of Transition Metal Selenides for Electrochemical Oxygen Reduction to Hydrogen Peroxide: From Catalyst Design to Electrolyzers Application DOI
Yingnan Wang,

Caidi Han,

Li Ma

et al.

Small, Journal Year: 2024, Volume and Issue: 20(22)

Published: Feb. 16, 2024

Abstract Hydrogen peroxide (H 2 O ) is a highly value‐added and environmental‐friendly chemical with various applications. The production of H by electrocatalytic 2e − oxygen reduction reaction (ORR) has emerged as promising alternative to the energy‐intensive anthraquinone process. High selectivity Catalysts combining superior activity are critical for efficient electrosynthesis . Earth‐abundant transition metal selenides (TMSs) being discovered classic stable, low‐cost, active selective catalysts electrochemical ORR. These features come from relatively large atomic radius selenium element, metal‐like properties abundant reserves. Moreover, compared advanced noble or single‐atom catalysts, kinetic current density TMSs generation higher in acidic solution, which enable them become suitable catalyst candidates. Herein, recent progress ORR systematically reviewed. effects electrocatalysts on activity, stability summarized. It intended provide an insight design corresponding mechanisms device setup, discuss relationship between structure activity.

Language: Английский

Citations

22
Identification of Cu0/Cu+/Cu0 interface as superior active sites for CO2 electroreduction to C2+ in neutral condition DOI
Xi Cao, Shan Ren, Xue Zhang

et al.

Chem, Journal Year: 2024, Volume and Issue: 10(7), P. 2089 - 2102

Published: March 15, 2024

Language: Английский

Citations

21
Fluorine Doping‐Assisted Reconstruction of Isolated Cu Sites for CO2 Electroreduction Toward Multicarbon Products DOI Creative Commons
Chen Jia, Xin Tan, Qian Sun

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 19, 2025

Abstract The electrocatalytic synthesis of multicarbon compounds from CO 2 is a promising method for storing renewable electricity and addressing global issues. Single‐atom catalysts are candidates reduction, but producing high‐value (C 2+ ) products using single‐atom structure remains significant challenge. In this study, fluorine doping strategy proposed to facilitate the reconstruction isolated Cu atoms, promoting generation. in situ formed nanocrystals contain substantial amount stable + species, demonstrating remarkable activity −to‐multicarbon conversion. Notably, they achieve highest utilization, with C partial current density −2.01 A mg per −1 formation rate 7.03 mmol h at ≈−1 V versus RHE. Raman spectroscopy functional theory calculations confirm crucial role atoms structural evolution electrolysis.

Language: Английский

Citations

5