Understanding the structure-performance relationship of active sites at atomic scale

Nano Research, Год журнала: 2022, Номер 15(8), С. 6888 - 6923

Опубликована: Июнь 14, 2022

Язык: Английский

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Oxygen Vacancy-Mediated Selective C–N Coupling toward Electrocatalytic Urea Synthesis

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(26), С. 11530 - 11535

Опубликована: Июнь 24, 2022

The electrocatalytic C-N coupling for one-step urea synthesis under ambient conditions serves as the promising alternative to traditional synthetic protocol. However, hydrogenation of intermediate species hinders efficient synthesis. Herein, oxygen vacancy-enriched CeO2 was demonstrated electrocatalyst with stabilization crucial *NO via inserting into vacant sites, which is conducive subsequent process rather than protonation, whereas poor selectivity protonation observed on vacancy-deficient catalyst. vacancy-mediated selective distinguished and validated by in situ sum frequency generation spectroscopy. introduction vacancies tailors common catalyst carrier an a high yield rate 943.6 mg h-1 g-1, superior that partial noble-metal-based electrocatalysts. This work provides novel insights design developments systems.

Язык: Английский

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Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Год журнала: 2022, Номер 15(9), С. 7806 - 7839

Опубликована: Июнь 2, 2022

Язык: Английский

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Electrocatalytic Hydrogenation of 5‐Hydroxymethylfurfural Promoted by a Ru₁Cu Single‐Atom Alloy Catalyst

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(37)

Опубликована: Июль 25, 2022

Electrochemical reduction of biomass-derived 5-hydroxymethylfurfural (HMF) represents an elegant route toward sustainable value-added chemicals production that circumvents the use fossil fuel and hydrogen. However, reaction efficiency is hampered by high voltage low activity electrodes (Cu, Bi, Pb). Herein, we report a Ru1 Cu single-atom alloy (SAA) catalyst with isolated Ru atoms on nanowires exhibits electrochemical HMF to 2,5-dihydroxymethylfuran (DHMF) promoted productivity (0.47 vs. 0.08 mmol cm-2 h-1 ) faradic (FE) (85.6 71.3 %) at -0.3 V (vs. RHE) compared counterpart. More importantly, FE (87.5 largely retained concentration (100 mM). Kinetic studies using combined techniques suggest disparate mechanisms over Cu, revealing promotes dissociation water produce H* species effectively react via electrocatalytic hydrogenation (ECH) mechanism.

Язык: Английский

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Accelerating electrochemical CO2 reduction to multi-carbon products via asymmetric intermediate binding at confined nanointerfaces

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Март 9, 2023

Abstract Electrochemical CO 2 reduction (CO R) to ethylene and ethanol enables the long-term storage of renewable electricity in valuable multi-carbon (C 2+ ) chemicals. However, carbon–carbon (C–C) coupling, rate-determining step R C conversion, has low efficiency poor stability, especially acid conditions. Here we find that, through alloying strategies, neighbouring binary sites enable asymmetric binding energies promote -to-C electroreduction beyond scaling-relation-determined activity limits on single-metal surfaces. We fabricate experimentally a series Zn incorporated Cu catalysts that show increased CO* surface coverage for fast C–C coupling consequent hydrogenation under electrochemical Further optimization reaction environment at nanointerfaces suppresses hydrogen evolution improves utilization acidic achieve, as result, high 31 ± 2% single-pass yield mild-acid pH 4 electrolyte with >80% efficiency. In single flow cell electrolyzer, realize combined performance 91 Faradaic notable 73 efficiency, full-cell energy 24 1% conversion commercially relevant current density 150 mA cm −2 over h.

Язык: Английский

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Isolating Single and Few Atoms for Enhanced Catalysis

Advanced Materials, Год журнала: 2022, Номер 34(39)

Опубликована: Май 17, 2022

Abstract Atomically dispersed metal catalysts have triggered great interest in the field of catalysis owing to their unique features. Isolated single or few atoms can be anchored on substrates via chemical bonding space confinement maximize atom utilization efficiency. The key challenge lies precisely regulating geometric and electronic structure active centers, thus significantly influencing catalytic properties. Although several reviews been published preparation, characterization, application single‐atom (SACs), comprehensive understanding SACs, dual‐atom (DACs), atomic clusters has never systematically summarized. Here, recent advances engineering local environments state‐of‐the‐art DACs, for enhanced performance are highlighted. Firstly, various synthesis approaches presented. Then, special attention is focused elucidation terms state coordination structure. Furthermore, a summary isolated applications thermocatalysis, electrocatalysis, photocatalysis provided. Finally, potential challenges future opportunities this emerging This review will pave way regulate microenvironment site boosting processes.

Язык: Английский

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Electrochemical CO₂reduction to C₂₊products using Cu-based electrocatalysts: A review

Deleted Journal, Год журнала: 2022, Номер 1, С. e9120021 - e9120021

Опубликована: Июль 4, 2022

With the disruptive carbon cycle being blamed for global warming, plausible electrocatalytic CO₂ reduction reaction (CO₂RR) to form valuable C₂₊ hydrocarbons and feedstock is becoming a hot topic. Cu-based electrocatalysts have been proven be excellent CO₂RR alternatives high energy value-added products in this regard. However, selectivity of via catalysts suffers from overpotential, slow kinetics, low selectivity. This review attempts discuss various cutting-edge strategies understanding catalytic design such as catalyst surface engineering, tuning Cu bandgap alloying, nanocatalysis, effect electrolyte pH on morphology. The most recent advances in situ spectroscopy computational techniques are summarized fully comprehend mechanisms, structural transformation/degradation crystal facet loss with subsequent effects activity. Furthermore, approaches interactions discussed four key perspectives: single-atom catalysts, interfacial metal-organic frameworks, polymer-incorporated materials, which provide new insights into products. Finally, major challenges outlined, potential prospects rational robust proposed. integration mechanistic step forward promising advancement technology industrial applications.

Язык: Английский

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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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Delocalization state-induced selective bond breaking for efficient methanol electrosynthesis from CO2

Nature Catalysis, Год журнала: 2022, Номер 6(1), С. 6 - 15

Опубликована: Дек. 12, 2022

Язык: Английский

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Recent Advances in Electrocatalysts for Efficient Nitrate Reduction to Ammonia

Advanced Functional Materials, Год журнала: 2023, Номер 33(43)

Опубликована: Июнь 25, 2023

Abstract Ammonia as an irreplaceable chemical has been widely demanded to keep the sustainable development of modern society. However, its industrial production consumes huge energy and releases extraordinary green‐house gases, leading various environmental issues. To achieve green ammonia is a great challenge that extensively pursued recently. In review, most promising strategy, electrochemical nitrate reduction reaction (e‐NO 3 RR) for purpose comprehensively investigated give full understanding mechanism provide guidance future directions. Particularly, electrocatalysts focused realize high yield rate Faraday efficiency applications. The recent‐developed catalysts, including noble metallic materials, alloys, metal compounds, single‐metal‐atom metal‐free are systematically discussed review effects factors on catalytic performance in e‐NO RR. Accordingly, strategies, defects engineering, coordination environment modulating, surface controlling, hybridization, carefully improve performance, such intrinsic activity selectivity. Finally, perspectives challenges given out. This shall insightful advanced systems efficiently industry.

Язык: Английский

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