Cascade Electrocatalytic and Thermocatalytic Reduction of CO2 to Propionaldehyde DOI
Jie Zhang,

Xingsi Kang,

Yuchen Yan

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(12)

Published: Jan. 18, 2024

Abstract Electrochemical CO 2 reduction can convert to value‐added chemicals, but its selectivity toward C 3+ products are very limited. One possible solution is run the reactions in hybrid processes by coupling electrocatalysis with other catalytic routes. In this contribution, we report cascade electrocatalytic and thermocatalytic of propionaldehyde. Using Cu(OH) nanowires as precatalyst, /H O reduced concentrated H 4 , CO, gases a zero‐gap membrane electrode assembly (MEA) reactor. The thermochemical hydroformylation reaction separately investigated series rhodium‐phosphine complexes. best candidate identified be one 1,4‐bis(diphenylphosphino)butane diphosphine ligand, which exhibits propionaldehyde turnover number 1148 under mild temperature close‐to‐atmospheric pressure. By optimizing upstream electroreduction downstream reaction, achieve ~38 % total 3 oxygenate 44 based on . These values represent more than seven times improvement over prior electrochemical system alone or two systems.

Language: Английский

Membrane Electrode Assembly for Electrocatalytic CO2 Reduction: Principle and Application DOI
Zheng Zhang, Xin Huang, Zhou Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(28)

Published: March 27, 2023

Abstract Electrocatalytic CO 2 reduction reaction (CO RR) in membrane electrode assembly (MEA) systems is a promising technology. Gaseous can be directly transported to the cathode catalyst layer, leading enhanced rate. Meanwhile, there no liquid electrolyte between and anode, which help improve energy efficiency of whole system. The remarkable progress achieved recently points out way realize industrially relevant performance. In this review, we focus on principles MEA for RR, focusing gas diffusion electrodes ion exchange membranes. Furthermore, anode processes beyond oxidation water are considered. Besides, voltage distribution scrutinized identify specific losses related individual components. We also summarize generation different reduced products together with corresponding catalysts. Finally, challenges opportunities highlighted future research.

Language: Английский

Citations

97
Tandem reactors and reactions for CO2 conversion DOI Creative Commons
Samay Garg, Zhenhua Xie, Jingguang G. Chen

et al.

Nature Chemical Engineering, Journal Year: 2024, Volume and Issue: 1(2), P. 139 - 148

Published: Feb. 8, 2024

Carbon dioxide (CO2) valorization is a promising pathway for mitigating greenhouse gas emissions from the chemical sector and reducing reliance of manufacturing on fossil fuel feedstocks. This Perspective discusses tandem catalytic paradigms sustainable CO2 conversion that have potential advantages over processes using single-functional catalysts. Recent progress discussed catalysis multifunctional catalysts in single reactor, as well reactors involving multiple Opportunities further developing these strategies thermochemical electrochemical various configurations are presented to encourage research this burgeoning field. Tandem provide unique opportunities sustainably converting into valuable products not accessible by traditional processes. process involve combinations thermocatalysis, electrocatalysis, photocatalysis, plasma biocatalysis.

Language: Английский

Citations

27
Recent Progress on Copper‐Based Bimetallic Heterojunction Catalysts for CO2 Electrocatalysis: Unlocking the Mystery of Product Selectivity DOI
Jiabao Huang,

Xinping Zhang,

Yang Jiao

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(24)

Published: April 18, 2024

Abstract Copper‐based bimetallic heterojunction catalysts facilitate the deep electrochemical reduction of CO 2 (eCO RR) to produce high‐value‐added organic compounds, which hold significant promise. Understanding influence copper interactions with other metals on adsorption strength various intermediates is crucial as it directly impacts reaction selectivity. In this review, an overview formation mechanism catalytic products in eCO RR provided and highlight uniqueness copper‐based catalysts. By considering different metals' tendencies toward intermediates, are classified, including copper, into four categories. The significance advantages constructing then discussed delve research findings current development status types Finally, insights offered design strategies for future high‐performance electrocatalysts, aiming contribute multi‐carbon fuels high

Language: Английский

Citations

15
Cascade Electrocatalytic and Thermocatalytic Reduction of CO2 to Propionaldehyde DOI
Jie Zhang,

Xingsi Kang,

Yuchen Yan

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(12)

Published: Jan. 18, 2024

Abstract Electrochemical CO 2 reduction can convert to value‐added chemicals, but its selectivity toward C 3+ products are very limited. One possible solution is run the reactions in hybrid processes by coupling electrocatalysis with other catalytic routes. In this contribution, we report cascade electrocatalytic and thermocatalytic of propionaldehyde. Using Cu(OH) nanowires as precatalyst, /H O reduced concentrated H 4 , CO, gases a zero‐gap membrane electrode assembly (MEA) reactor. The thermochemical hydroformylation reaction separately investigated series rhodium‐phosphine complexes. best candidate identified be one 1,4‐bis(diphenylphosphino)butane diphosphine ligand, which exhibits propionaldehyde turnover number 1148 under mild temperature close‐to‐atmospheric pressure. By optimizing upstream electroreduction downstream reaction, achieve ~38 % total 3 oxygenate 44 based on . These values represent more than seven times improvement over prior electrochemical system alone or two systems.

Language: Английский

Citations

13
Plasma Chemical Looping: Unlocking High-Efficiency CO2 Conversion to Clean CO at Mild Temperatures DOI Creative Commons

Yanhui Long,

Xingzi Wang, Hai Zhang

et al.

JACS Au, Journal Year: 2024, Volume and Issue: 4(7), P. 2462 - 2473

Published: May 8, 2024

We propose a plasma chemical looping CO

Language: Английский

Citations

13
Bimetallic-Derived Catalytic Structures for CO2-Assisted Ethane Activation DOI
Zhenhua Xie, Jingguang G. Chen

Accounts of Chemical Research, Journal Year: 2023, Volume and Issue: 56(18), P. 2447 - 2458

Published: Aug. 30, 2023

ConspectusIn recent years, the simultaneous upgrading of CO2 and ethane has emerged as a promising approach for generating valuable gaseous (CO, H2, ethylene) liquid (aromatics C3 oxygenates) chemicals from greenhouse gas large-reserved shale gas. The key challenges controlling product selectivity lie in selective C-H C-C bond cleavage with assistance CO2. Bimetallic-derived catalysts likely undergo alloying or oxygen-induced segregation under reaction conditions, thus providing diverse types interfacial sites, e.g., metal/support (M/M'Ox) interface metal oxide/metal (M'Ox/M) inverse interface, that are beneficial CO2-assisted upgrading. extent can be initially predicted by cohesive energy atomic radius (or Wigner-Seitz radius), while preference to form on-top suboxide approximated using work function, electronegativity, binding strength adsorbed oxygen. Furthermore, bimetallic-derived typically supported on high surface area oxides. Modifying reducibility acidity/basicity oxide supports introducing defects facilitate activation oxygen supplies activation.Using situ synchrotron characterization density functional theory (DFT) calculations, we found electronic properties species influence C-H/C-C bonds ethane, electron-deficient over alloy) promoting nonselective scission produce syngas electron-enriched enhancing yield ethylene. We further demonstrate preferred structures catalyst surfaces, either alloy surfaces interfaces, controlled through appropriate choice combinations their ratios. Through comprehensive comparison experimental results DFT C-C/C-H is correlated thermodynamically favorable (i.e., interfaces) conditions wide range bimetallic catalysts. These findings not only offer structural mechanistic insights into but also provide design principles other light alkanes. This Account concludes discussing opportunities designing advanced catalysts, incorporating new chemistries products, employing precise synthesis strategies well-defined optimized site densities, leveraging time/spatial/energy-resolved spectroscopy/scattering/microscopy techniques analysis. research methodologies established here helpful investigation dynamic should inspire more efforts toward

Language: Английский

Citations

21
Direct HCN synthesis via plasma-assisted conversion of methane and nitrogen DOI Creative Commons
Nefeli S. Kamarinopoulou, Gerhard R. Wittreich, Dionisios G. Vlachos

et al.

Science Advances, Journal Year: 2024, Volume and Issue: 10(13)

Published: March 29, 2024

Hydrogen cyanide (HCN) is synthesized from ammonia (NH 3 ) and methane (CH 4 at ~ 1200°C over a Pt catalyst. Ammonia synthesis entails several complex, highly emitting processes. Plasma-assisted HCN directly CH nitrogen (N 2 could be pivotal for on-demand production. Here, we evaluate the potential of dielectric barrier discharge (DBD) N /CH plasma decentralized catalyst-free selective We demonstrate single-step conversion to with 72% yield <300°C. favored low concentrations ethane (C H 6 as secondary product. propose first-principles microkinetic model few electron impact reactions. The accurately predicts primary product yields elucidates that methyl radical (·CH common intermediate in C synthesis. Compared current industrial processes, DBD can achieve minimal CO emissions.

Language: Английский

Citations

8
Membrane Electrode Assembly for Electrocatalytic CO2 Reduction: Principle and Application DOI
Zheng Zhang, Xin Huang, Zhou Chen

et al.

Angewandte Chemie, Journal Year: 2023, Volume and Issue: 135(28)

Published: March 27, 2023

Abstract Electrocatalytic CO 2 reduction reaction (CO RR) in membrane electrode assembly (MEA) systems is a promising technology. Gaseous can be directly transported to the cathode catalyst layer, leading enhanced rate. Meanwhile, there no liquid electrolyte between and anode, which help improve energy efficiency of whole system. The remarkable progress achieved recently points out way realize industrially relevant performance. In this review, we focus on principles MEA for RR, focusing gas diffusion electrodes ion exchange membranes. Furthermore, anode processes beyond oxidation water are considered. Besides, voltage distribution scrutinized identify specific losses related individual components. We also summarize generation different reduced products together with corresponding catalysts. Finally, challenges opportunities highlighted future research.

Language: Английский

Citations

15
Tandem Electrocatalytic–Thermocatalytic Conversion of CO2 to Aromatic Hydrocarbons DOI
Samay Garg, Zhenhua Xie,

Alexandria X. Lam

et al.

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(6), P. 2990 - 2996

Published: May 28, 2024

The reaction of CO2 with H2O to produce aromatic hydrocarbons (benzene, toluene, ethylbenzene, and xylene isomers) (BTEX) represents a promising pathway for converting value-added liquid products. However, this cannot be achieved in single electrochemical or thermochemical process. This work utilizes tandem electrochemical–thermochemical reactors as new paradigm by starting the feed membrane electrode assembly (MEA) C2H4, which subsequently undergoes aromatization using gallium- phosphorus-modified zeolite ZSM-5 catalyst (Ga/ZSM-5/P) at ambient pressure BTEX. current study also demonstrates potential advantage strategy mitigating negative effects water testing reactor system under different hydration conditions performing situ X-ray diffraction (XRD) absorption (XAS) characterization catalysts. These results highlight process use trap before reactor.

Language: Английский

Citations

6
Advanced systems for enhanced CO2 electroreduction DOI
Wenfu Xie, Bingkun Li, Lu Liu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 4, 2024

This review explores the latest developments in CO 2 electroreduction based systems, including coupling reaction co-reduction cascade and integrated capture conversion systems.

Language: Английский

Citations

6