Steering the Site Distance of Atomic Cu‐Cu Pairs by First‐Shell Halogen Coordination Boosts CO2‐to‐C2 Selectivity DOI

Fengya Ma,

Pengfang Zhang,

Xiaobo Zheng

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(46)

Published: Aug. 6, 2024

Abstract Electrocatalytic reduction of CO 2 into C products high economic value provides a promising strategy to realize resourceful utilization. Rational design and construct dual sites the protonation C−C coupling unravel their structure‐performance correlation is great significance in catalysing electrochemical reactions. Herein, Cu−Cu with different site distance coordinated by halogen at first‐shell are constructed shows higher intramolecular electron redispersion coordination symmetry configurations. The long‐range (Cu−I−Cu) show an enhanced Faraday efficiency products, up 74.1 %, excellent stability. In addition, linear relationships that accelerated H 4 generation short‐range (Cu−Cl−Cu) beneficial for 5 OH formation disclosed. situ attenuated total reflection surface infrared absorption spectroscopy, Raman theoretical calculations manifest can weaken reaction energy barriers hydrogenation coupling, as well accelerating deoxygenation *CH CHO. This study uncovers exploitation site‐distance‐dependent properties steer pathway, potential generic tactic target synthesis constructing desired sites.

Language: Английский

Steering the Reconstruction of Oxide-Derived Cu by Secondary Metal for Electrosynthesis of n-Propanol from CO DOI
Chang Long, Kaiwei Wan, Yu Chen

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(7), P. 4632 - 4641

Published: Feb. 10, 2024

As fuel and an important chemical feedstock, n-propanol is highly desired in electrochemical CO2/CO reduction on Cu catalysts. However, the precise regulation of localized structure still challenging poorly understood, thus hindering selective electrosynthesis. Herein, by decorating Au nanoparticles (NPs) CuO nanosheets (NSs), we present a counterintuitive transformation into undercoordinated sites locally around NPs during CO reduction. In situ spectroscopic techniques reveal Au-steered formation abundant removal oxygen CuO. First-principles accuracy molecular dynamic simulation demonstrates that atoms tend to rearrange disordered layer rather than (111) close-packed plane observed bare NSs. These facilitate binding, enabling electroreduction with high Faradaic efficiency 48% flow cell. This work provides new insight oxide-derived catalysts reconstruction secondary metal component.

Language: Английский

Citations

26
Steering the Site Distance of Atomic Cu‐Cu Pairs by First‐Shell Halogen Coordination Boosts CO2‐to‐C2 Selectivity DOI Open Access

Fengya Ma,

Pengfang Zhang,

Xiaobo Zheng

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(46)

Published: Aug. 6, 2024

Electrocatalytic reduction of CO

Language: Английский

Citations

20
In-depth understanding and precise modulation of surface reconstruction during heterogeneous electrocatalysis: From model to practical catalyst DOI
Weidong Dai, Kaiwei Wan, Kanglei Pang

et al.

Chem, Journal Year: 2025, Volume and Issue: 11(1), P. 102345 - 102345

Published: Jan. 1, 2025

Language: Английский

Citations

4
Ultralow Coordination Copper Sites Compartmentalized within Ordered Pores for Highly Efficient Electrosynthesis of n-Propanol from CO2 DOI
Qun Li, Jiabin Wu, Caoyu Yang

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 25, 2025

Coordinatively unsaturated copper (Cu) has been demonstrated to be effective for electrifying CO2 reduction into C3 products by adjusting the coupling of C1-C2 intermediates. Nevertheless, intuitive impacts ultralow coordination Cu sites on are scarcely elucidated due lack synthetic recipes with low numbers and its vulnerability aggregation under reductive potentials. Herein, computational predictions revealed that higher levels coordinative unsaturation favored adsorption C1 C2 Building upon correlations, we constructed an catalyst from in situ oxide nanoparticles (CuO NPs) compartmentalized within ordered porous matrix, achieving a remarkable Faradaic efficiency (FE) n-propanol (n-PrOH) electroreduction, reaching up 27.4% H-cell at -0.8 VRHE 11.8% 300 mA cm-2 flow cell. The presence maintenance during rigorous electrolysis process contributed outstanding performances, as verified combination spectroscopy techniques, disclosing formed featured strong *C1 *C2 intermediates lead n-PrOH.

Language: Английский

Citations

3
Direct Electrochemical Reduction of CO2 to C2+ Chemicals: Catalysts, Microenvironments, and Mechanistic Understanding DOI
Shichen Guo, J. Wang, Haozhe Zhang

et al.

ACS Energy Letters, Journal Year: 2025, Volume and Issue: 10(1), P. 600 - 619

Published: Jan. 2, 2025

The electrochemical reduction reaction of CO2 (eCO2RR) to chemicals presents a viable solution for addressing climate change and sustainable manufacturing. In this Review, we describe the recent advancements in eCO2RR multicarbon (C2+) production from aspects catalyst structure, microenvironments, mechanistic understanding. We draw experimental theoretical comparisons between systems containing bulk highly dispersed metals, alloys, metal compounds recount new results microenvironmental impacts as well catalytic mechanism. From our own studies, offer some viewpoints on electrocatalytic mechanism during complex multistep proton-coupled electron transfers propose several research directions unlocking full potential scalable industrial CO2-to-C2+ conversion.

Language: Английский

Citations

2
Promoting Water Activation via Molecular Engineering Enables Efficient Asymmetric C–C Coupling during CO2 Electroreduction DOI

Zi‐Yu Du,

Si-Bo Li,

Ge-Hao Liang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(47), P. 32870 - 32879

Published: Nov. 13, 2024

Water activation plays a crucial role in CO

Language: Английский

Citations

13
Synthesis and Electrocatalytic Applications of Layer‐Structured Metal Chalcogenides Composites DOI
Yongteng Qian, Fangfang Zhang,

Xiaohui Luo

et al.

Small, Journal Year: 2024, Volume and Issue: 20(26)

Published: Jan. 14, 2024

Abstract Featured with the attractive properties such as large surface area, unique atomic layer thickness, excellent electronic conductivity, and superior catalytic activity, layered metal chalcogenides (LMCs) have received considerable research attention in electrocatalytic applications. In this review, approaches developed to synthesize LMCs‐based electrocatalysts are summarized. Recent progress composites for electrochemical energy conversion applications including oxygen reduction reaction, carbon dioxide evolution hydrogen overall water splitting, nitrogen reaction is reviewed, potential opportunities practical obstacles development of high‐performing active substances also discussed. This review may provide an inspiring guidance developing high‐performance LMCs

Language: Английский

Citations

12
Electrocatalytic upcycling of plastic waste: Progress, challenges, and future DOI Creative Commons
Jinzhou Li, J.T. Chen, Luyao Zhang

et al.

Electron, Journal Year: 2024, Volume and Issue: 2(3)

Published: Aug. 1, 2024

Abstract The escalating accumulation of plastic waste has been developed into a formidable global environmental challenge. Traditional disposal methods such as landfilling and incineration not only exacerbate degradation by releasing harmful chemicals greenhouse gases, but also squander finite resources that could otherwise be recycled or repurposed. Upcycling is kind recycling technology converts high‐value helps to avoid resource pollution. Electrocatalytic upcycling emerges novel distinguished its mild operational conditions, high transformation efficiency product selectivity. This review commences with an overview the employed in management respective advantages inherent limitations are delineated. different types upcycled electrocatalytic strategy then discussed process examined together mechanisms underlying upcycling. Furthermore, structure‐activity relationships between electrocatalysts performance elucidated. aims furnish readers comprehensive understanding techniques for provide guidance design towards efficient transformation.

Language: Английский

Citations

12
Recent advances in copper-based catalysts for electrocatalytic CO 2 reduction toward multi-carbon products DOI Creative Commons

Qiang Wang,

Hehe Wei, Ping Liu

et al.

Deleted Journal, Journal Year: 2024, Volume and Issue: 3(3), P. e9120112 - e9120112

Published: Jan. 18, 2024

Electrocatalytic carbon dioxide reduction reaction (CO2RR) holds the promise of both overcoming greenhouse effect and synthesizing a wealth chemicals. CO2 toward carbon-containing products, including C1 products (carbon monoxide, formic acid, etc), C2 (ethylene, ethanol, etc.) multi-carbon (e.g., npropanol), provides beneficial fuel chemicals for industrial production. The complexity multi-proton transfer processes difficulties C-C coupling in electrochemical multi-carbon(C2+) have attracted increasing concerns on design catalysts comparison with those products. In this paper, we review main advances syntheses through electrocatalytic recent years, introduce basic principles CO2RR, detailly elucidate two widely accepted mechanisms reactions. Among abundant nanomaterials, copper-based are outstanding preparation CO2RR attributing to effective Regarding different selectivity but extensively applied catalysts, classify summarize various Cu-based separating diverse where modification spatial electronic structures is increase coverage CO or lower activation energy barrier forming CC bond form key intermediates production Challenges prospects involving fundamental development also proposed.

Language: Английский

Citations

11
Robust imidazole-linked Ni-phthalocyanine-based covalent-organic framework for CO2 electroreduction in full pH range DOI

Xu Yang,

Duan‐Hui Si, Hongfang Li

et al.

Materials Chemistry Frontiers, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

Ni-phthalocyanine-based covalent-organic framework linked by imidazole group exhibits brilliant stability and high activity of CO 2 electroreduction reaction with over 90% Faradic efficiency in full pH range.

Language: Английский

Citations

10