Membrane Electrode Assembly for Electrocatalytic CO₂ Reduction: Principle and Application

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(28)

Опубликована: Март 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.

Язык: Английский

---

Tandem reactors and reactions for CO2 conversion

Nature Chemical Engineering, Год журнала: 2024, Номер 1(2), С. 139 - 148

Опубликована: Фев. 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.

Язык: Английский

---

Recent Progress on Copper‐Based Bimetallic Heterojunction Catalysts for CO₂ Electrocatalysis: Unlocking the Mystery of Product Selectivity

Advanced Science, Год журнала: 2024, Номер 11(24)

Опубликована: Апрель 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

Язык: Английский

---

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

JACS Au, Год журнала: 2024, Номер 4(7), С. 2462 - 2473

Опубликована: Май 8, 2024

We propose a plasma chemical looping CO

Язык: Английский

---

Cascade Electrocatalytic and Thermocatalytic Reduction of CO₂ to Propionaldehyde

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(12)

Опубликована: Янв. 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.

Язык: Английский

---

Bimetallic-Derived Catalytic Structures for CO₂-Assisted Ethane Activation

Accounts of Chemical Research, Год журнала: 2023, Номер 56(18), С. 2447 - 2458

Опубликована: Авг. 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

Язык: Английский

---

Direct HCN synthesis via plasma-assisted conversion of methane and nitrogen

Science Advances, Год журнала: 2024, Номер 10(13)

Опубликована: Март 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.

Язык: Английский

---

Membrane Electrode Assembly for Electrocatalytic CO₂ Reduction: Principle and Application

Angewandte Chemie, Год журнала: 2023, Номер 135(28)

Опубликована: Март 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.

Язык: Английский

---

Tandem Electrocatalytic–Thermocatalytic Conversion of CO₂ to Aromatic Hydrocarbons

ACS Energy Letters, Год журнала: 2024, Номер 9(6), С. 2990 - 2996

Опубликована: Май 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.

Язык: Английский

---

CO₂ Conversion to Butene via a Tandem Photovoltaic–Electrochemical/Photothermocatalytic Process: A Co-design Approach to Coupled Microenvironments

ACS Energy Letters, Год журнала: 2024, Номер 9(9), С. 4369 - 4377

Опубликована: Авг. 15, 2024

We developed a tandem, unassisted, solar-driven electrochemical and photothermocatalytic process for the single-pass conversion of CO2 to butene using only simulated solar irradiation as energetic input. The two-step involves reduction (CO2R) ethylene followed by dimerization butene. assessed two unassisted setups concentrate in CO2R reactor, achieving concentrations up 5.4 vol% with 1.8% average solar-to-ethylene 5.6% CO2-to-ethylene under 1-sun illumination. When effluent gas stream was passed through oligomerization we generated 600 ppm 3-sun Through analysis this process, identified that presence H2, CO, H2O leads rapid deactivation Ni-based catalyst.

Язык: Английский

---