Stabilizing the oxidation state of catalysts for effective electrochemical carbon dioxide conversion

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(12), P. 6295 - 6321

Published: Jan. 1, 2024

Developing sophisticated strategies to stabilize oxidative metal catalysts based on the correlation between dynamic oxidation state and product profile is favorable for efficient electrochemical CO 2 conversion.

Language: Английский

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Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Language: Английский

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Beyond Leverage in Activity and Stability toward CO₂ Electroreduction to Formate over a Bismuth Catalyst

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(10), P. 8050 - 8061

Published: May 8, 2024

The direct production of formate from CO2 over Bi-based catalysts offers a promising route for producing important chemicals using renewable electricity. Nevertheless, limited by the unstable structure and states under electrochemical conditions, electroreduction to is still facing trade-off between activity stability, especially at high current densities. Herein, we reported metal–carbon interfacial modulation strategy synthesize cross-linked defective carbon-modified Bi nanoparticle (Bi-DC) catalyst with stable spatial unique CO2-philic hydrophobic interface. As result, Bi-DC featured remarkable ability in near neutral electrolyte (1 M KHCO3) was even comparable CO2-to-formate strongly basic systems, along partial density formation rate −378 mA cm–2 7 mmol h–1, respectively. Also, it achieved electrolysis 120 h 0.4 A membrane electrode assembly reactor operated stably an industrial large 5 A. carbon species promoted reconstruction dispersion active component Bi, together confinement effect that facilitated long-term electrolysis.

Language: Английский

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Electrocatalytic membrane with p-block bismuth atoms for selective oxygen activation to hydroxyl radicals for effective water decontamination

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 352, P. 124044 - 124044

Published: April 21, 2024

Language: Английский

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Wearable Biodevices Based on Two-Dimensional Materials: From Flexible Sensors to Smart Integrated Systems

Nano-Micro Letters, Journal Year: 2025, Volume and Issue: 17(1)

Published: Jan. 15, 2025

Abstract The proliferation of wearable biodevices has boosted the development soft, innovative, and multifunctional materials for human health monitoring. integration sensors with intelligent systems is an overwhelming tendency, providing powerful tools remote monitoring personal management. Among many candidates, two-dimensional (2D) stand out due to several exotic mechanical, electrical, optical, chemical properties that can be efficiently integrated into atomic-thin films. While previous reviews on 2D primarily focus conventional configurations like graphene, rapid new opened up novel applications, particularly in smart interaction functionalities. This review aims consolidate recent progress, highlight unique advantages materials, guide future research by discussing existing challenges opportunities applying biodevices. We begin in-depth analysis advantages, sensing mechanisms, potential applications biodevice fabrication. Following this, we systematically discuss state-of-the-art based various physiological signals within body. Special attention given showcasing multi-functionality devices, mainly including self-power supply, diagnosis/treatment, human–machine interaction. Finally, concludes a concise summary prospective solutions concerning utilization advanced

Language: Английский

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Tip carbon encapsulation customizes cationic enrichment and valence stabilization for low K+ acidic CO2 electroreduction

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Feb. 19, 2025

Abstract Acidic electrochemical CO 2 conversion is a promising alternative to overcome the low utilization. However, over-reliance on highly concentrated K + inhibit hydrogen evolution reaction also causes (bi)carbonate precipitation interfere with catalytic performance. In this work, under screening and guidance of computational simulations, we present carbon coated tip-like O 3 electrocatalyst for stable efficient acidic synthesize formic acid (HCOOH) concentration. The layer protects oxidized species higher intrinsic activity from reductive corrosion, peripherally formulates tip-induced electric field regulate adverse H attraction desirable enrichment. an electrolyte at pH 0.94, only 0.1 M required achieve Faradaic efficiency (FE) 98.9% 300 mA cm −2 HCOOH long-time stability over100 h. By up-scaling electrode into 25 electrolyzer setup, total current 7 A recorded sustain durable production 291.6 mmol L −1 h .

Language: Английский

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Nanocluster Surface Microenvironment Modulates Electrocatalytic CO₂ Reduction

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(13)

Published: Dec. 19, 2023

The catalytic activity and product selectivity of the electrochemical CO

Language: Английский

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Selectivity of Electrochemical CO₂Reduction on Metal Electrodes: The Role of the Surface Oxidized Layer

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(19), P. 13089 - 13100

Published: Sept. 22, 2023

In the past decade, density functional theory (DFT) calculations have been employed to study mechanism of electrochemical CO2 reduction reactions. However, lack understanding chemisorption states, proton-coupled-electron-transfer (PCET) steps, and dynamic redox reactions electrode surface has limited reliability these simulations. The *OCHO *COOH species are widely recognized as key intermediates for formic acid carbon monoxide production, respectively. comparison between binding energies cannot directly indicate reaction trends. this work, we propose that energy difference on neutral extra-electron substrates, in form [ΔG(*COOHe) – ΔG(*COOH)], can serve a descriptor selectivity. addition, computational hydrogen (CHE) model is revised by applying previously studied charged species. noninteger charge-transfer (NICT) used calculation profile at certain potential, which good prediction potential-limiting step. oxide metal electrodes found play role modulating selectivity improving electron transfer CO2.

Language: Английский

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Leveraging Inherent Structure of Tin Oxide for Efficient Carbonaceous Products Electrosynthesis

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(33)

Published: June 27, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) holds a great potential for converting into valuable carbon‐based chemicals and fuels. A promising strategy enhancing RR performance is the deliberate structural design of electrocatalysts, which can maximize utilization inherent advantages. In this work, SnO nanocubes (NCs) nanorods (NRs) are synthesized using surface energy‐driven growth orientation method, where stable (110) facet highly energetic (001) constitute nanostructures. Leveraging merits different facets on , theoretical calculations reveal that plays primary role in inhibiting hydrogen evolution (HER), while both favorable ‐to‐formate conversion under external bias. As result, NCs with higher ratio (001)/(110) achieve nearly 100% selectivity formation carbonaceous products during RR. More importantly, maximum partial current density about 1 cm −2 formate Faradaic efficiency (FE) over 90% achieved flow cell, distinguishing it from most reported Sn‐based electrocatalysts. These results highlight strategic advantages leveraging structure nanomaterials efficient

Language: Английский

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Theoretical insights into lanthanide rare earth single-atom catalysts for electrochemical CO₂ reduction

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(26), P. 16183 - 16189

Published: Jan. 1, 2024

This study comprehensively investigated the catalytic performance of lanthanide rare earth metals (REMs) anchored into Salen for CO 2 RR in terms stability, selectivity, and activity using density functional theory (DFT).

Language: Английский

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