Fabrication of Ultrahigh‐Loading Dual Copper Sites in Nitrogen‐Doped Porous Carbons Boosting Electroreduction of CO2 to C2H4 Under Neutral Conditions DOI
Jin‐Meng Heng, Haolin Zhu, Zhen‐Hua Zhao

et al.

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

Published: Nov. 16, 2024

Abstract Synthesis of high‐loading atomic‐level dispersed catalysts for highly efficient electrochemical CO 2 reduction reaction (eCO RR) to ethylene (C H 4 ) in neutral electrolyte remain challenging tasks. To address common aggregation issues, a host‐guest strategy is employed, by using metal‐azolate framework ( MAF‐4 with nanocages as the host and dinuclear Cu(I) complex guest, form precursors pyrolysis into series nitrogen‐doped porous carbons (NPCs) varying loadings dual copper sites, namely NPC ‐Cu ‐21 (21.2 wt%), ‐11 (10.6 ‐7 (6.9 wt%). Interestingly, loading sites increased from 6.9 21.2 wt%, partial current density eCO RR yield C also gradually 38.7 93.6 mA cm −2 . In 0.1 m KHCO 3 electrolyte, at −1.4 V versus reversible hydrogen electrode vs RHE), exhibits excellent performance Faradaic efficiency 52% 180 Such can be attributed presence ultrahigh‐loading which promotes C─C coupling formation products. The findings demonstrate confinement effect conducive preparation catalysts.

Language: Английский

Electrocatalytic CO2 hydrogenation to C2+ alcohols catalysed by Pr–Cu oxide heterointerfaces DOI

J Liu,

Pengsong Li, Shuaiqiang Jia

et al.

Nature Synthesis, Journal Year: 2025, Volume and Issue: unknown

Published: March 13, 2025

Language: Английский

Citations

1
High Fe-Loading Single-Atom Catalyst Boosts ROS Production by Density Effect for Efficient Antibacterial Therapy DOI Creative Commons
Si Chen,

Fang Huang,

Lijie Mao

et al.

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 17(1)

Published: Oct. 4, 2024

Abstract The current single-atom catalysts (SACs) for medicine still suffer from the limited active site density. Here, we develop a synthetic method capable of increasing both metal loading and mass-specific activity SACs by exchanging zinc with iron. constructed iron (h 3 -FNC) high 6.27 wt% an optimized adjacent Fe distance ~ 4 Å exhibit excellent oxidase-like catalytic performance without significant decay after being stored six months promising antibacterial effects. Attractively, “density effect” has been found at high-enough doping amount, which individual sites become close enough to interact each other alter electronic structure, resulting in significantly boosted intrinsic single-atomic h -FNCs 2.3 times compared low- medium-loading SACs. Consequently, overall -FNC is highly improved, mass that are, respectively, 66 315 higher than those commercial Pt/C. In addition, demonstrate efficiently enhanced capability catalyzing oxygen reduction into superoxide anion (O 2 · − ) glutathione (GSH) depletion. Both vitro vivo assays superior efficacy promoting wound healing. This work presents intriguing activity-enhancement effect exhibits impressive therapeutic combating bacterial infections.

Language: Английский

Citations

8
Regulating the Critical Intermediates of Dual‐Atom Catalysts for CO2 Electroreduction DOI
Mengyang Zhang,

Dingyang Zhou,

Xueqin Mu

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: May 27, 2024

Electrocatalysis is a very attractive way to achieve sustainable carbon cycle by converting CO

Language: Английский

Citations

7
Radiation‐Synthesized Metal–Organic Frameworks with Ligand‐Induced Lewis Pairs for Selective CO2 Electroreduction DOI
Wenhui Liu, Bijun Tang, Kai Huang

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 15, 2024

Abstract The electrochemical activation of inert CO 2 molecules through C─C coupling reactions under ambient conditions remains a significant challenge but holds great promise for sustainable development and the reduction emission. Lewis pairs can capture react with , offering novel strategy electrosynthesis high‐value‐added C2 products. Herein, an electron‐beam irradiation is presented rapidly synthesizing metal–organic framework (MOF) well‐defined (i.e., Cu‐ N pyridinic ). synthesized MOFs exhibit total product faradic efficiency 70.0% at −0.88 V versus RHE. In situ attenuated reflection Fourier transform infrared Raman spectra reveal that electron‐deficient acidic Cu sites electron‐rich basic in ligand facilitate targeted chemisorption, activation, conversion molecules. DFT calculations further elucidate electronic interactions key intermediates reaction. work not only advances pair‐site as new platform conversion, also provides pioneering insights into underlying mechanisms irradiated synthesis advanced nanomaterials.

Language: Английский

Citations

7
Customizing catalyst surface/interface structures for electrochemical CO2 reduction DOI Creative Commons
Xin Tan, Haojie Zhu,

Chang He

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(12), P. 4292 - 4312

Published: Jan. 1, 2024

This review article summarizes the recent progress in customizing surface/interface structures for CO 2 RR electrocatalysts (including atomic-site catalysts, metal and metal/oxide catalysts).

Language: Английский

Citations

6
Electrocatalytic reduction of carbon dioxide to C4+ products DOI
Xiangyun Ma, Boon Siang Yeo

Current Opinion in Electrochemistry, Journal Year: 2024, Volume and Issue: 46, P. 101534 - 101534

Published: May 10, 2024

Language: Английский

Citations

6
Recent advances of metal-organic frameworks and MOF-derived materials based on p-block metal for the electrochemical reduction of carbon dioxide DOI
Xinyu Wu, Jianfeng Lu, Zihao Zhu

et al.

Chinese Chemical Letters, Journal Year: 2024, Volume and Issue: unknown, P. 110151 - 110151

Published: June 1, 2024

Language: Английский

Citations

6
Asymmetrically Coordinated Cu Dual‐Atom‐Sites Enables Selective CO2 Electroreduction to Ethanol DOI
Changli Chen,

Zhiyi Sun,

Gangzhi Qin

et al.

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

Published: Oct. 6, 2024

Abstract Electrochemical reduction of CO 2 (CO RR) to value‐added liquid fuels is a highly attractive solution for carbon‐neutral recycling, especially C 2+ products. However, the selectivity control preferable products great challenge due complex multi‐electron proton transfer process. In this work, series Cu atomic dispersed catalysts are synthesized by regulating coordination structures optimize RR selectivity. ‐SNC catalyst with uniquely asymmetrical coordinated CuN ‐CuNS site shows high ethanol selective FE 62.6% at −0.8 V versus RHE and 60.2% 0.9 in H‐Cell Flow‐Cell test, respectively. Besides, nest‐like structure beneficial mass process selection catalytic situ experiments theory calculations reveal reaction mechanisms such ethanol. The S atoms weaken bonding ability adjacent carbon atom, which accelerates from *CHCOH generate *CHCHOH, resulting This work indicates promising strategy rational design asymmetrically single, dual, or tri‐atom provides candidate material produce

Language: Английский

Citations

6
Experimental and Theoretical Insights into Single Atoms, Dual Atoms, and Sub‐Nanocluster Catalysts for Electrochemical CO2 Reduction (CO2RR) to High‐Value Products DOI Creative Commons
Abebe Reda Woldu, Asfaw G. Yohannes, Zanling Huang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(52)

Published: Nov. 26, 2024

Abstract Electrocatalytic carbon dioxide (CO 2 ) conversion into valuable chemicals paves the way for realization of recycling. Downsizing catalysts to single‐atom (SACs), dual‐atom (DACs), and sub‐nanocluster (SNCCs) has generated highly active selective CO transformation reduced products. This is due introduction numerous sites, unsaturated coordination environments, efficient atom utilization, confinement effect compared their nanoparticle counterparts. Herein, recent Cu‐based SACs are first reviewed newly emerged DACs SNCCs expanding catalysis electrocatalytic reduction RR) high‐value products discussed. Tandem SAC–nanocatalysts (NCs) (SAC–NCs) also discussed RR Then, non‐Cu‐based SACs, DACs, SAC–NCs, theoretical calculations various transition‐metal summarized. Compared previous achievements less‐reduced products, this review focuses on double objective achieving full increasing selectivity formation rate toward C–C coupled with additional emphasis stability catalysts. Finally, through combined experimental research, future outlooks offered further develop over isolated atoms sub‐nanometal clusters.

Language: Английский

Citations

6
Mesostructure‐Specific Configuration of *CO Adsorption for Selective CO2 Electroreduction to C2+ Products DOI

Zaiqi Li,

Bin Sun,

Difei Xiao

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(1)

Published: Sept. 2, 2024

The multi-carbon (C2+) alcohols produced by electrochemical CO2 reduction, such as ethanol and n-propanol, are considered indispensable liquid energy carriers. In most C-C coupling cases, however, the concomitant gaseous C2H4 product results in low selectivity of C2+ alcohols. Here, we report rational construction mesostructured CuO electrocatalysts, specifically mesoporous (m-CuO) cylindrical (c-CuO), enables selective distribution products. m-CuO c-CuO show similar towards total products (≥76 %), but corresponding predominant (55 %) (52 respectively. ordered mesostructure not only induces surface hydrophobicity, selectively tailors adsorption configuration *CO intermediate: prefers bridged adsorption, whereas favors top revealed situ spectroscopies. Computational calculations unravel that adsorbate is prone to deep protonation into *OCH3 intermediate, thus accelerating intermediates generate alcohols; contrast, apt undergo conventional process produce C2H4. This work illustrates via manipulation, paves a new path design efficient electrocatalysts with tunable key for targeted

Language: Английский

Citations

5