Electroreduction of CO₂: Advances in the Continuous Production of Formic Acid and Formate

ACS Energy Letters, Год журнала: 2023, Номер 8(4), С. 1992 - 2024

Опубликована: Март 30, 2023

The study of the electrochemical CO2 reduction to obtain formate (HCOO–) or formic acid (HCOOH) is receiving much attention as a promising technology. Since continuous–mode operation has become necessary for practical implementation reduction, recent years have seen rapid increase in number research approaches focusing on this aspect. This Focus Review provides unified discussion available studies continuous electroreduction HCOO–/HCOOH, considering different important features process design. Moreover, paper quantitatively assesses performance that involve reactors converting HCOOH/HCOO–, comparing relevant typically used figures merit, including energy consumption. Although some trade-offs already been achieved, simultaneous optimization all merit remains challenge. Finally, concluding remarks highlight detected trends and discuss aspects will be tackled by future field.

Язык: Английский

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Stabilizing indium sulfide for CO2 electroreduction to formate at high rate by zinc incorporation

Nature Communications, Год журнала: 2021, Номер 12(1)

Опубликована: Окт. 5, 2021

Recently developed solid-state catalysts can mediate carbon dioxide (CO2) electroreduction to valuable products at high rates and selectivities. However, under commercially relevant current densities of > 200 milliamperes per square centimeter (mA cm-2), often undergo particle agglomeration, active-phase change, and/or element dissolution, making the long-term operational stability a considerable challenge. Here we report an indium sulfide catalyst that is stabilized by adding zinc in structure shows dramatically improved stability. The obtained ZnIn2S4 reduce CO2 formate with 99.3% Faradaic efficiency 300 mA cm-2 over 60 h continuous operation without decay. By contrast, similarly synthesized participation deteriorates quickly same conditions. Combining experimental theoretical studies, unveil introduction largely enhances covalency In-S bonds, which "locks" sulfur-a catalytic site activate H2O react CO2, yielding HCOO* intermediates-from being dissolved during high-rate electrolysis.

Язык: Английский

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BiPO₄‐Derived 2D Nanosheets for Efficient Electrocatalytic Reduction of CO₂ to Liquid Fuel

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(14), С. 7681 - 7685

Опубликована: Янв. 15, 2021

Abstract The electrochemical reduction of carbon dioxide (CO 2 ) to high‐value liquid fuel with high selectivity is appealing for energy conversion and storage. Here we report a bismuth phosphate (BiPO 4 derived 2D nanosheet‐like electrocatalyst that efficiently converts CO into liquid‐phase formate. catalyst presents formate Faradaic efficiency over 90 % cathodic 73 at an industrially relevant current density 200 mA cm −2 in the flow cell. situ generation Bi‐O active species on surface was determined via operando Raman measurement. Morphological X‐ray photoelectron spectroscopy analyses reveal origin activity electrosynthesis from water: structure together abundant insertion oxygen atoms BiPO ‐derived nanosheets.

Язык: Английский

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Bi₂O₃/BiO₂ Nanoheterojunction for Highly Efficient Electrocatalytic CO₂ Reduction to Formate

Nano Letters, Год журнала: 2022, Номер 22(4), С. 1656 - 1664

Опубликована: Фев. 4, 2022

Heterostructure engineering plays a vital role in regulating the material interface, thus boosting electron transportation pathway advanced catalysis. Herein, novel Bi2O3/BiO2 heterojunction catalyst was synthesized via molten alkali-assisted dealumination strategy and exhibited rich structural dynamics for an electrocatalytic CO2 reduction reaction (ECO2RR). By coupling situ X-ray diffraction Raman spectroscopy measurements, we found that as-synthesized heterostructure can be transformed into Bi/BiO2 Mott–Schottky heterostructure, leading to enhanced adsorption performance *OCHO intermediates. Consequently, high selectivity toward formate larger than 95% rendered wide potential window along with optimum partial current density of −111.42 mA cm–2 benchmarked state-of-the-art Bi-based ECO2RR catalysts. This work reports construction fruitful dynamic insights electrocatalyst ECO2RR, which paves way rational design efficient electrocatalysts beyond.

Язык: Английский

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Bismuth-based metal–organic frameworks and their derivatives: Opportunities and challenges

Coordination Chemistry Reviews, Год журнала: 2021, Номер 439, С. 213902 - 213902

Опубликована: Март 24, 2021

Язык: Английский

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Spontaneously Sn-Doped Bi/BiO_x Core–Shell Nanowires Toward High-Performance CO₂ Electroreduction to Liquid Fuel

Nano Letters, Год журнала: 2021, Номер 21(16), С. 6907 - 6913

Опубликована: Авг. 9, 2021

Electrochemical CO2 reduction provides a promising strategy to product value-added fuels and chemical feedstocks. However, it remains grand challenge further reduce the overpotentials increase current density for large-scale applications. Here, spontaneously Sn doped Bi/BiOx nanowires (denoted as Bi/Bi(Sn)Ox NWs) with core–shell structure were synthesized by an electrochemical dealloying strategy. The NWs exhibit impressive formate selectivity over 92% from −0.5 −0.9 V versus reversible hydrogen electrode (RHE) achieve of 301.4 mA cm–2 at −1.0 vs RHE. In-situ Raman spectroscopy theoretical calculations reveal that introduction atoms into BiOx species can promote stabilization *OCHO intermediate on Bi(Sn)Ox surface suppress competitive H2/CO production. This work effective in situ construction metal/metal oxide hybrid composites heteroatom doping new insights promoting conversion practical

Язык: Английский

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Anode Catalysts in CO₂ Electrolysis: Challenges and Untapped Opportunities

ACS Catalysis, Год журнала: 2022, Номер 12(2), С. 1037 - 1051

Опубликована: Янв. 4, 2022

The field of electrochemical carbon dioxide reduction has developed rapidly during recent years. At the same time, role anodic half-reaction received considerably less attention. In this Perspective, we scrutinize reports on best-performing CO2 electrolyzer cells from past 5 years, to shed light oxygen evolution catalyst. We analyze how different cell architectures provide local chemical environments at anode surface, which in turn determines pool applicable catalysts. uncover factors that led either a strikingly high current density operation or an exceptionally long lifetime. On basis our analysis, set criteria have be fulfilled by catalyst achieve performance. Finally, outlook using alternative reactions (alcohol oxidation is discussed as example), resulting high-value products and higher energy efficiency for overall process.

Язык: Английский

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Applications of Metal–Organic Frameworks and Their Derivatives in Electrochemical CO2 Reduction

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Апрель 30, 2023

Abstract Electrochemically reducing CO 2 to more reduced chemical species is a promising way that not only enables the conversion of intermittent energy resources stable fuels, but also helps build closed-loop anthropogenic carbon cycle. Among various electrocatalysts for electrochemical reduction, multifunctional metal–organic frameworks (MOFs) have been employed as highly efficient and selective heterogeneous due their ultrahigh porosity topologically diverse structures. Up now, great progress has achieved in design synthesis active MOF-related catalysts reduction reaction (CO RR), corresponding mechanisms thoroughly studied. In this review, we summarize recent applying MOFs derivatives RR, with focus on strategies electrolyzers. We first discussed different RR products introduced commonly applied electrolyzer configurations current system. Then, an overview several categories (CO, HCOOH, CH 4 , 3 OH, multi-carbon chemicals) generated from or via was discussed. Finally, offer some insights perspectives future development reduction. aim provide new into field further guide research large-scale applications.

Язык: Английский

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Enabling heterogeneous catalysis to achieve carbon neutrality: Directional catalytic conversion of CO₂ into carboxylic acids

Carbon Energy, Год журнала: 2023, Номер 6(3)

Опубликована: Май 25, 2023

Abstract The increase in anthropogenic carbon dioxide (CO 2 ) emissions has exacerbated the deterioration of global environment, which should be controlled to achieve neutrality. Central core goal achieving neutrality is utilization CO under economic and sustainable conditions. Recently, strong need for led a proliferation studies on direct conversion into carboxylic acids, can effectively alleviate create high‐value chemicals. purpose this review present application prospects acids basic principles through photo‐, electric‐, thermal catalysis. Special attention focused regulation strategy activity abundant catalysts at molecular level, inspiring preparation high‐performance catalysts. In addition, theoretical calculations, advanced technologies, numerous typical examples are introduced elaborate corresponding process influencing factors catalytic activity. Finally, challenges provided future development field. It hoped that will contribute deeper understanding inspire more innovative breakthroughs.

Язык: Английский

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Emerging bismuth-based materials: From fundamentals to electrochemical energy storage applications

Energy storage materials, Год журнала: 2023, Номер 58, С. 232 - 270

Опубликована: Март 23, 2023

Язык: Английский

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