Enhancing Local CO₂ Adsorption by L‐histidine Incorporation for Selective Formate Production Over the Wide Potential Window

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(49)

Опубликована: Окт. 19, 2023

Electrochemical carbon dioxide reduction reaction (CO2 RR) to produce valuable chemicals is a promising pathway alleviate the energy crisis and global warming issues. However, simultaneously achieving high Faradaic efficiency (FE) current densities of CO2 RR in wide potential range remains as huge challenge for practical implements. Herein, we demonstrate that incorporating bismuth-based (BH) catalysts with L-histidine, common amino acid molecule proteins, an effective strategy overcome inherent trade-off between activity selectivity. Benefiting from significantly enhanced adsorption capability promoted electron-rich nature by L-histidine integrity, BH catalyst exhibits excellent FEformate unprecedented windows (>90 % within -0.1--1.8 V >95 -0.2--1.6 versus reversible hydrogen electrode, RHE). Excellent performance can still be achieved under low-concentration feeding (e.g., 20 vol.%). Besides, extremely low onset -0.05 VRHE (close theoretical thermodynamic -0.02 ) was detected situ ultraviolet-visible (UV-Vis) measurements, together stable operation over 50 h preserved ≈95 partial density 326.2 mA cm-2 at -1.0 .

Язык: Английский

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Selective capture of uranium by p-block bismuth-based metal–organic framework

Desalination, Год журнала: 2024, Номер 576, С. 117360 - 117360

Опубликована: Янв. 22, 2024

Язык: Английский

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Advances in Sn-based oxide catalysts for the electroreduction of CO2 to formate

Green Carbon, Год журнала: 2024, Номер 2(2), С. 131 - 148

Опубликована: Апрель 17, 2024

The excessive consumption of fossil fuels increases CO2 emissions, and the consequent greenhouse effect resulting from higher levels this gas in atmosphere has a significant impact on environment climate. This necessitated development environmentally friendly efficient methods for conversion. carbon dioxide electroreduction reaction (CO2RR), which is driven by electricity generated renewable energy sources (e.g., wind solar) to convert into value-added or chemicals, regarded as promising prospective path toward cycling. Among various products, formate, with its relatively simple preparation process, broad application prospects, can be used fuel, hydrogen storage material, raw material downstream chemicals. Sn-based oxide electrocatalysts have advantages being inexpensive nontoxic. In addition, these catalysts offer high product selectivity are electrochemical reduction formate. review, we first clarify mechanisms factors that influence then provide some examples technologies could study evolution during reaction. particular, focus traditional oxides (SnO2) novel perovskite been developed use field CO2RR recent years considering their synthesis, catalytic performance, optimization strategies, intrinsic principles. Finally, current challenges opportunities discussed. perspectives latest trends presented review expected inspire researchers contribute more efforts comprehensively optimizing performance produce

Язык: Английский

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MOF-Based Electrocatalysts: An Overview from the Perspective of Structural Design

Chemical Reviews, Год журнала: 2025, Номер unknown

Опубликована: Фев. 18, 2025

The electrocatalytic technique, as an efficient energy storage and conversion technology, has attracted significant attention to address exhaustion environmental pollution. Usually, the activity selectivity of reactions are largely dominated by dynamic process occurring on electrocatalysts. Therefore, high-performance electrocatalysts, which can dominate pathway barrier reactions, great significance for advancement technique. Metal-organic frameworks (MOFs), emerging crystalline porous materials, present structural component advantages including well-defined structure, high surface area, large porosity, diverse components, easy tailorability, demonstrating fantastic potential precise fabrication In this Review, strategies in electrocatalysts based MOF-related materials specifically introduced from aspects catalytic site design microenvironment modulation around sites. Furthermore, representative progress achieved various applications employing MOF-based is systematically summarized, with special emphasis MOFs performance optimization. Finally, remaining challenges future perspectives further highlighted.

Язык: Английский

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Anion Modulation of Ag‐Imidazole Cuboctahedral Cage Microenvironments for Efficient Electrocatalytic CO2 Reduction

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(31)

Опубликована: Май 20, 2024

How to achieve CO

Язык: Английский

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Catalytic Dechlorination of Three Organochlorides by Recyclable Nano-Palladium-Engineered Natural Sponge with Formic Acid

Catalysts, Год журнала: 2024, Номер 14(7), С. 424 - 424

Опубликована: Июль 3, 2024

Catalytic dechlorination of organic chlorides by palladium (Pd) with HCOOH represents one the most effective and promising techniques for environmental remediation. In this study, we adopted alkaline-modified porous natural sponge as support a Pd nanocatalyst (Pd@M-Sponge) hydrogen source hydrodechlorination florfenicol (FF), o-chlorophenol (o-CP), p-chlorophenol (p-CP). Favorable conversion efficiency FF, o-CP, p-CP was achieved at 25 °C atmospheric pressure attributed to small diameter high catalytic reactivity prepared NPs, in addition slight internal mass transfer limitation Pd@M-Sponge. High reaction rate constants were obtained even conditions low molar ratio (10:1) concentration (500 mg/L). The catalyst also demonstrated superior recyclability without any obvious decrease 20 successive cycles. This work provides an ideal recyclable cost-effective based on renewable biocompatible material chlorinated pollutants formic acid new view exploration designing highly reactive stable catalysts hydrodechlorination.

Язык: Английский

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Value‐Added Cascade Synthesis Mediated by Paired‐Electrolysis Using an Ultrathin Microenvironment‐Inbuilt Metalized Covalent Organic Framework Heterojunction

Advanced Energy Materials, Год журнала: 2024, Номер 14(27)

Опубликована: Апрель 25, 2024

Abstract Energy‐saving and value‐added management in advanced catalysis is highly desirable but challenged by the limitations of multifunctional catalysts catalytic modules. Herein, an azo‐linked phthalocyanine‐porphyrin covalent organic framework (COF) with ultrathin layered nanostructure grown on carbon nanotubes (NiPc‐azo‐H2Pp@CNTs) has been designed synthesized, which can serve as a active stable bifunctional heterojunction electrocatalyst for selective paired‐electrosynthesis through coupling anodic iodide oxidation reaction cathodic CO 2 conversion. Particularly, inbuilt local microenvironment conferred dihydroporphyrin moieties COF act proton reservoir to promote relay at interface during electrocatalytic process. Moreover, cascade construction dual electrocatalytic/organocatalytic modules, cathode‐generated be further converted dimethyl carbonate yield 6.21 mmol L −1 h , while anode‐produced iodine derived into iodoform hundred‐milligram scale. It worth noting that synthesis mediated paired‐electrolysis using distinctive high‐powered electrocatalysts will help advance sustainable development industrial intelligent manufacturing.

Язык: Английский

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Overview on Building Blocks and Applications of Efficient and Robust Extended Tight Binding

The Journal of Physical Chemistry A, Год журнала: 2025, Номер unknown

Опубликована: Фев. 27, 2025

The extended tight binding (xTB) family of methods opened many new possibilities in the field computational chemistry. Within just 5 years, GFN2-xTB parametrization for all elements up to Z = 86 enabled more than a thousand applications, which were previously not feasible with other electronic structure methods. xTB provide robust and efficient way apply quantum mechanics-based approaches obtaining molecular geometries, computing free energy corrections or describing noncovalent interactions found applicability targets. A crucial contribution success is availability within simulation packages frameworks, supported by open source development its program library packages. We present comprehensive summary applications capabilities different fields Moreover, we consider main software calculations, covering their current ecosystem, novel features, usage scientific community.

Язык: Английский

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Tuning strategies and electrolyzer design for Bi-based nanomaterials towards efficient CO2 reduction to formic acid

Chinese Journal of Structural Chemistry, Год журнала: 2024, Номер 43(8), С. 100346 - 100346

Опубликована: Май 21, 2024

Язык: Английский

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Tuning the local coordination environment of silver(I) coordination networks with counterions for enhanced electrocatalytic CO2 reduction

Science China Chemistry, Год журнала: 2024, Номер 67(5), С. 1524 - 1530

Опубликована: Фев. 4, 2024

Язык: Английский

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