Electronic Delocalization of Bismuth Oxide Induced by Sulfur Doping for Efficient CO₂ Electroreduction to Formate

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(12), P. 7604 - 7612

Published: June 9, 2021

Developing efficient electrocatalysts for electrochemical CO2 reduction (ECR) to fuels and chemicals with high product faradaic efficiency (FE) current density is desirable but remains challenging. Herein, S-doped Bi2O3 coupled carbon nanotubes (S-Bi2O3-CNT) are synthesized ECR formate. The obtained S2-Bi2O3-CNT (with a S doping amount of 0.7 at. %) highly active formate production (FE > 90%) over wide range (2.77–48.6 mA cm–2), maximum FE 97.06% can be achieved at −0.9 V. significantly enhanced selectivity activity originated from the fast electron transfer, adsorption, more undercoordinated Bi sites induced by doping. More importantly, functional theory calculations revealed that lead an electronic delocalization Bi, which benefits binding *CO2 *HCOO ECR, while inhibiting hydrogen evolution reaction via weakening adsorption *H, thus helping achieve FE. This work paves promising way tuning activities atomic level.

Language: Английский

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Process modeling, techno-economic assessment, and life cycle assessment of the electrochemical reduction of CO2: a review

iScience, Journal Year: 2021, Volume and Issue: 24(7), P. 102813 - 102813

Published: July 1, 2021

The electrochemical reduction of CO2 has emerged as a promising alternative to traditional fossil-based technologies for the synthesis chemicals. Its industrial implementation could lead in carbon footprint chemicals and mitigation climate change impacts caused by hard-to-decarbonize applications, among other benefits. However, current low technology readiness levels such emerging make it hard predict their performance at scales. During past few years, researchers have developed diverse techniques model assess toward its implementation. aim this literature review is provide comprehensive overview techno-economic life cycle assessment methods pave way future approaches. First, we identify which modeling approaches been conducted extend analysis production scale. Next, explore metrics used evaluate systems, regarding technical, environmental, economic aspects. Finally, challenges research opportunities via electrolysis.

Language: Английский

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Atomic-level insights into surface engineering of semiconductors for photocatalytic CO2 reduction

Journal of Energy Chemistry, Journal Year: 2021, Volume and Issue: 67, P. 309 - 341

Published: Oct. 25, 2021

Photocatalytic conversion of CO2 into solar fuels provides a bright route for the green and sustainable development human society. However, realization efficient photocatalytic reduction reaction (CO2RR) is still challenging owing to sluggish kinetics or unfavorable thermodynamics basic chemical processes CO2RR, such as adsorption, activation, product desorption. To overcome these shortcomings, recent works have demonstrated that surface engineering semiconductors, introducing vacancy, doping, cocatalyst loading, serves effective promising strategies improved CO2RR with high activity selectivity. The essential reason lies in activation pathways can be optimized regulated through reconstruction atomic electronic structures. Herein, this review, we focus on research advances about rational design semiconductor CO2RR. selectivity will reviewed. In addition, theoretical calculations along situ characterization techniques spotlight clarify process. aim review provide deep understanding guidance semiconductors

Language: Английский

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Guiding CO₂RR Selectivity by Compositional Tuning in the Electrochemical Double Layer

Accounts of Chemical Research, Journal Year: 2022, Volume and Issue: 55(4), P. 504 - 515

Published: Feb. 4, 2022

ConspectusThe electrochemical conversion of carbon dioxide to value-added chemicals provides an environmentally benign alternative current industrial practices. However, electrocatalytic systems for the CO2 reduction reaction (CO2RR) are not practical industrialization, owing poor specific product selectivity and/or limited activity. Interfacial engineering presents a versatile and effective method direct CO2RR by fine-tuning local chemical dynamics. This Account describes interfacial design strategies developed in our laboratory that use electrolyte porous materials modify composition at electrode–electrolyte interface.Our first strategy influencing surface reactivity is perturb double layer tuning composition. We approached this investigation considering how charged molecular additives can organize electrode impact activation. Using combination advanced techniques situ vibrational spectroscopy, we show surfactant properties (the identity headgroup, alkyl chain length, concentration) as well cation affect molecules assemble biased electrode. The interplay between cations be regulated favor products, such HCOO–, suppress parasitic hydrogen evolution (HER). Together, findings highlight assemblies used selective systems.In addition design, spatial confinement intermediates another selectivity. were interested uncovering role carbon-supported catalysts toward formation. In initial study, porosity optimized enhance C2H4 CO series Cu embedded tunable aerogel matrix. These results suggested active plays activation motivated into probing phenomenon translated planar Our modifiers facilitated reconstruction diffusion HER improve C2–3 Given ubiquity catalysis, work demonstrates regulating restricting substrate intermediates. increased potential versatility boosting catalytic performance across array systems.

Language: Английский

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Lignin‐Based Materials for Additive Manufacturing: Chemistry, Processing, Structures, Properties, and Applications

Advanced Science, Journal Year: 2023, Volume and Issue: 10(9)

Published: Jan. 19, 2023

Abstract The utilization of lignin, the most abundant aromatic biomass component, is at forefront sustainable engineering, energy, and environment research, where its abundance low‐cost features enable widespread application. Constructing lignin into material parts with controlled desired macro‐ microstructures properties via additive manufacturing has been recognized as a promising technology paves way to practical application lignin. Considering rapid development significant progress recently achieved in this field, comprehensive critical review outlook on three‐dimensional (3D) printing highly desirable. This article fulfils demand an overview structure presents state‐of‐the‐art 3D pristine lignin‐based composites, highlights key challenges. It attempted deliver better fundamental understanding impacts morphology, microstructure, physical, chemical, biological modifications, composition/hybrids rheological behavior lignin/polymer blends, well as, mechanical, chemical performance printed materials. main points toward future developments involve hybrid manufacturing, situ polymerization, surface tension or energy driven molecular segregation are also elaborated discussed promote high‐value

Language: Английский

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Revisiting the Role of Discharge Products in Li–CO₂ Batteries

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(49)

Published: May 12, 2023

Abstract Rechargeable lithium‐carbon dioxide (Li–CO 2 ) batteries are promising devices for CO recycling and energy storage. However, thermodynamically stable electrically insulating discharge products (DPs) (e.g., Li 3 deposited at cathodes require rigorous conditions completed decomposition, resulting in large recharge polarization poor battery reversibility. Although progress has been achieved cathode design electrolyte optimization, the significance of DPs is generally underestimated. Therefore, it necessary to revisit role Li–CO boost overall performance. Here, a critical systematic review reported first time. Fundamentals reactions formation decomposition appraised; impacts on performance including overpotential, capacity, stability demonstrated; necessity product management highlighted. Practical situ/operando technologies assessed characterize reaction intermediates corresponding mechanism investigation. Additionally, achievable control measures evidenced provide principles improve Findings from this work will deepen understanding electrochemistry promote practical applications.

Language: Английский

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Recent advance of nanomaterials modified electrochemical sensors in the detection of heavy metal ions in food and water

Food Chemistry, Journal Year: 2023, Volume and Issue: 440, P. 138213 - 138213

Published: Dec. 16, 2023

Language: Английский

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Low-coordinated copper facilitates the *CH2CO affinity at enhanced rectifying interface of Cu/Cu2O for efficient CO2-to-multicarbon alcohols conversion

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 18, 2024

Abstract The carbon−carbon coupling at the Cu/Cu 2 O Schottky interface has been widely recognized as a promising approach for electrocatalytic CO conversion into value-added alcohols. However, limited selectivity of C 2+ alcohols persists due to insufficient control over rectifying characteristics required precise bonding oxyhydrocarbons. Herein, we present an investigation manipulation coordination environment Cu sites through in-situ electrochemical reconstruction strategy, which indicates that construction low-coordinated facilitates enhanced interfaces, and induces asymmetric electronic perturbation faster electron exchange, thereby boosting C-C oxyhydrocarbons towards nucleophilic reaction process *H CCO-CO. Impressively, exhibit superior faradic efficiency 64.15 ± 1.92% energy ~39.32% production, while maintaining stability 50 h (faradic >50%, total current density = 200 mA cm −2 ) in flow-cell electrolyzer. Theoretical calculations, operando synchrotron radiation Fourier transform infrared spectroscopy, Raman experiments decipher can enhance coverage *CO adsorption *CH CH CHO, facilitating formation

Language: Английский

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Reactive capture and electrochemical conversion of CO₂ with ionic liquids and deep eutectic solvents

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(17), P. 8563 - 8631

Published: Jan. 1, 2024

Ionic liquids (ILs) and deep eutectic solvents (DESs) have tremendous potential for reactive capture of CO 2 , due to their highly properties, including a wide electrochemical stability window, low volatility, high solubility.

Language: Английский

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Cu-based materials for electrocatalytic CO2 to alcohols: Reaction mechanism, catalyst categories, and regulation strategies

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 97, P. 593 - 611

Published: June 17, 2024

Language: Английский

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