Dual‐Metal Sites Drive Tandem Electrocatalytic CO2 to C2+ Products DOI Open Access

Guixian Xie,

Weiwei Guo,

Zijian Fang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(47)

Published: Aug. 14, 2024

Abstract The electrochemical conversion of CO 2 into valuable chemicals is a promising route for renowable energy storage and the mitigation greenhouse gas emission, production multicarbon (C 2+ ) products highly desired. Here, we report 1.4 %Pd−Cu@CuPz comprising dispersive CuO x PdO dual nanoclusters embedded in MOF CuPz (Pz=Pyrazole), which achieves high C Faradaic efficiency (FE C2+ 81.9 % alcohol FE 47.5 with remarkable stability when using 0.1 M KCl aqueous solution as electrolyte typical H‐cell. Particularly, obviously improved on compared to Cu@CuPz . Theoretical calculations have revealed that enhanced interfacial electron transfer facilitates adsorption *CO intermediate *CO−*CO dimerization Cu−Pd sites bridged by Cu nodes Additionally, oxophilicity Pd can stabilize key *CH CHO promote subsequent proton‐coupled more efficiently, confirming formation pathway skew towards *C H 5 OH. Consequently, play synergistic tandem role cooperatively improving selectivity accelerating reductive

Language: Английский

Emerging MOFs, COFs, and their derivatives for energy and environmental applications DOI Creative Commons
Xinyue Zhang, Mengfan Yan,

Pei Chen

et al.

The Innovation, Journal Year: 2025, Volume and Issue: 6(2), P. 100778 - 100778

Published: Jan. 18, 2025

Traditional fossil fuels significantly contribute to energy supply, economic development, and advancements in science technology. However, prolonged extensive use of has resulted increasingly severe environmental pollution. Consequently, it is imperative develop new, clean, pollution-free sources with high density versatility as substitutes for conventional fuels, although this remains a considerable challenge. Simultaneously, addressing water pollution critical concern. The design, optimization functional nanomaterials are pivotal advancing new solutions pollutant remediation. Emerging porous framework materials such metal-organic frameworks (MOFs) covalent organic (COFs), recognized exemplary crystalline materials, exhibit potential applications due their specific surface area, adjustable pore sizes structures, permanent porosity, customizable functionalities. This work provides comprehensive systematic review the MOFs, COFs, derivatives emerging technologies, including oxygen reduction reaction, evolution hydrogen lithium-ion batteries, remediation carbon dioxide reaction management. In addition, strategies performance adjustment structure-effect relationships these explored. Interaction mechanisms summarized based on experimental discussions, theoretical calculations, advanced spectroscopy analyses. challenges, future prospects, opportunities tailoring presented.

Language: Английский

Citations

23

Nanocavity enriched CuPd alloy with high selectivity for CO2 electroreduction toward C2H4 DOI
Ze-Yu Zhang, Haibin Wang,

Fei-Fei Zhang

et al.

Rare Metals, Journal Year: 2024, Volume and Issue: 43(4), P. 1513 - 1523

Published: Jan. 20, 2024

Language: Английский

Citations

19

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

18

Enhanced CO2 Electroreduction Selectivity toward Ethylene on Pyrazolate-Stabilized Asymmetric Ni–Cu Hybrid Sites DOI
Liang Huang, Ziao Liu, Ge Gao

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(48), P. 26444 - 26451

Published: Nov. 22, 2023

Metal-organic frameworks (MOFs) possess well-defined, designable structures, holding great potential in enhancing product selectivity for electrochemical CO2 reduction (CO2R) through active site engineering. Here, we report a novel MOF catalyst featuring pyrazolate-stabilized asymmetric Ni/Cu sites, which not only maintains structural stability under harsh conditions but also exhibits extraordinarily high ethylene (C2H4) during CO2R. At cathode of -1.3 V versus RHE, our catalyst, denoted as Cu1Ni-BDP, manifests C2H4 Faradaic efficiency (FE) 52.7% with an overall current density 0.53 A cm-2 1.0 M KOH electrolyte, surpassing that on prevailing Cu-based catalysts. More remarkably, the Cu1Ni-BDP stable performance 4.5% FE 25 h electrolysis. suite characterization tools─such high-resolution transmission electron microscopy, X-ray absorption spectroscopy, operando diffraction, and infrared spectroscopy─and functional theory calculations collectively reveal cubic pyrazolate-metal coordination structure Ni-Cu sites synergistically facilitate formation from CO2.

Language: Английский

Citations

42

Ligand Design in Atomically Precise Copper Nanoclusters and Their Application in Electrocatalytic Reactions DOI
Yuping Liu, Jinli Yu,

Yongfeng Lun

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(44)

Published: July 2, 2023

Abstract Metal nanoclusters (MNCs) are compositionally well‐defined and also structurally precise materials with unique molecule‐like properties discrete electronic energy levels. Atomically ligand‐protected Cu (LP‐CuNCs) one category of typical MNCs that usually demonstrate geometric structures to serve as electrocatalysts. However, the synthesis, application, well structure‐performance relationship LP‐CuNCs not adequately studied. Significantly, ligands essential structure, crystal size, structure LP‐CuNCs, which determine their physiochemical applications. In this review, significant progress in ligand design application electrocatalytic reactions is introduced. The general basics (LP‐MNCs) first introduced functions emphasized. Subsequently, a series different for including thiolates, phosphines, alkynyl, polymers, biomolecules highlighted. Thereafter, applications discussed. It believed review will only inspire synthesis novel but contribute extension establishment accurate relationships.

Language: Английский

Citations

37

Alloy Catalysts for Electrocatalytic CO2 Reduction DOI

Lizhen Liu,

Hossein Akhoundzadeh,

Mingtao Li

et al.

Small Methods, Journal Year: 2023, Volume and Issue: 7(9)

Published: May 31, 2023

Abstract CO 2 conversion is an anticipated route to resolve the energy crisis and environmental pollution, in which electrocatalysis one of technologies closest industrialization. Alloy catalysts are promising candidates for electrocatalysis, high tenability electronic structures surface physical chemical properties allows alloy catalytic activity selectivity electrocatalytic reduction. Herein, recent advances reduction have been systematically summarized, with insight into structure active center, performance, mechanism, uncover key their performance. The mainly classified as binary multi‐metallic alloys (medium entropy alloy) based on components mixed configuration entropy, relationship among mechanism has fully discussed inspire rational design catalysts. Finally, current challenges future perspectives presented propose dilemma development direction This review provides overview about progress present a guideline research work relevant

Language: Английский

Citations

35

Polymer Modification Strategy to Modulate Reaction Microenvironment for Enhanced CO2 Electroreduction to Ethylene DOI

Ting Deng,

Shuaiqiang Jia, Chunjun Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(2)

Published: Nov. 28, 2023

Abstract Modulation of the microenvironment on electrode surface is one effective means to improve efficiency electrocatalytic carbon dioxide reduction (eCO 2 RR). To achieve high conversion rates, phase boundary at should be finely controlled overcome limitation CO solubility in aqueous electrolyte. Herein, we developed a simple and efficient method structure electrocatalyst with superhydrophobic by one‐step co‐electrodeposition Cu polytetrafluoroethylene (PTFE) paper. The super‐hydrophobic Cu‐based displayed ethylene (C H 4 ) selectivity Faraday (FE) 67.3 % −1.25 V vs. reversible hydrogen (RHE) an H‐type cell, which 2.5 times higher than regular without PTFE. By using PTFE as modifier, activity eCO RR enhanced water (proton) adsorption inhibited. This strategy has potential applied other gas‐conversion electrocatalysts.

Language: Английский

Citations

24

Structuring Cu Membrane Electrode for Maximizing Ethylene Yield from CO2 Electroreduction DOI
Jianyu Han, Bin Tu, Pengfei An

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(21)

Published: Feb. 20, 2024

Electrocatalytic ethylene (C

Language: Английский

Citations

17

Stabilization of Cu+ sites by amorphous Al2O3 to enhance electrochemical CO2 reduction to C2+ products DOI

Hailian Cheng,

Shuaiqiang Jia,

Jiapeng Jiao

et al.

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(5), P. 2599 - 2604

Published: Jan. 1, 2024

The stabilized amorphous Al 2 O 3 phase stabilizes the Cu + site through oxidation state control, thereby improving selectivity and activity for production of C 2+ product.

Language: Английский

Citations

16

sp2-c linked Cu-based metal-covalent organic framework for chemical and photocatalysis synergistic reduction of uranium DOI
Jinlan Liu,

Mu-Xiang Lin,

Juan Huang

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 491, P. 151982 - 151982

Published: May 6, 2024

Language: Английский

Citations

14