Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond

Advanced Materials, Год журнала: 2023, Номер 36(17)

Опубликована: Июнь 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Язык: Английский

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Defect engineering of two-dimensional materials for advanced energy conversion and storage

Chemical Society Reviews, Год журнала: 2023, Номер 52(5), С. 1723 - 1772

Опубликована: Янв. 1, 2023

Defective two-dimensional (2D) materials show huge potential for energy-related fields. This review overviews the formation/evolution mechanisms and engineering strategies of defects in 2D materials, which enable enhanced electrode reaction kinetics.

Язык: Английский

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Local reaction environment in electrocatalysis

Chemical Society Reviews, Год журнала: 2024, Номер 53(4), С. 2022 - 2055

Опубликована: Янв. 1, 2024

Beyond conventional electrocatalyst engineering, recent studies have unveiled the effectiveness of manipulating local reaction environment in enhancing performance electrocatalytic reactions. The general principles and strategies environmental engineering for different processes been extensively investigated. This review provides a critical appraisal advancements aiming to comprehensively assess this emerging field. It presents interactions among surface structure, ions distribution electric field relation environment. Useful protocols such as interfacial reactant concentration, mass transport rate, adsorption/desorption behaviors, binding energy are in-depth discussed toward modifying Meanwhile, electrode physical structures cell configurations viable optimization methods environments. In combination with

Язык: Английский

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Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Год журнала: 2024, Номер 18(14), С. 9823 - 9851

Опубликована: Март 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Язык: Английский

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Bimetallic nanoalloys planted on super-hydrophilic carbon nanocages featuring tip-intensified hydrogen evolution electrocatalysis

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Авг. 21, 2024

The insufficient availability and activity of interfacial water remain a major challenge for alkaline hydrogen evolution reaction (HER). Here, we propose an "on-site disruption near-site compensation" strategy to reform the bonding network via deliberate cation penetration catalyst support engineering. This concept is validated using tip-like bimetallic RuNi nanoalloys planted on super-hydrophilic high-curvature carbon nanocages (RuNi/NC). Theoretical simulations suggest that tip-induced localized concentration hydrated K+ facilitates optimization dynamics intermediate adsorption. In situ synchrotron X-ray spectroscopy endorses H* spillover-bridged Volmer‒Tafel mechanism synergistically relayed between Ru Ni. Consequently, RuNi/NC exhibits low overpotential 12 mV high durability 1600 h at 10 mA cm‒2 HER, demonstrates performance in both electrolysis chlor-alkali electrolysis. offers microscopic perspective design manipulation local structure toward enhanced HER kinetics. A with optimized H2 reported. designed shows catalytic by achieving 13.6-fold higher mass than Pt/C.

Язык: Английский

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The Missing Link for Electrochemical CO₂ Reduction: Classification of CO vs HCOOH Selectivity via PCA, Reaction Pathways, and Coverage Analysis

ACS Catalysis, Год журнала: 2024, Номер 14(4), С. 2151 - 2161

Опубликована: Янв. 26, 2024

For the electrochemical CO2 reduction reaction, different metal catalysts preferentially produce products. However, differences between metals' reaction pathways that lead to these products are still not fully understood. In this work, we analyze CO vs HCOOH formation from using statistical analysis and density functional theory calculations. This is carried out by considering multiple descriptors, along with competing pathways, barriers, high coverage of mixed adsorbates on surface. method capable explaining discrepancy simulations experiments regarding Ag Au selectivity properly classifying elements according their product distribution. We find that, when water-assisted protonation for disproportionation CO, have a lower barrier production in agreement experimental results. also surfaces, most stable adsorbate configuration contains forming preferentially. These findings help bridge gap provide missing link our understanding reaction.

Язык: Английский

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Electrocatalytic Reduction of Carbon Dioxide to High-Value Multicarbon Products with Metal–Organic Frameworks and Their Derived Materials

ACS Materials Letters, Год журнала: 2022, Номер 4(11), С. 2058 - 2079

Опубликована: Сен. 26, 2022

The electrocatalytic carbon dioxide reduction reaction (CO2RR) holds great potential in promoting neutral through effectively converting CO2 molecules to useful chemicals and fuels. high-efficiency electrochemical conversion of single-carbon products has been well realized, while more efforts are needed for the generation high-value multicarbon products. Metal–organic frameworks (MOFs), featuring porous structures, high chemical tunability, ultralarge surface area, have attracted increasing attention CO2RR. Herein, we review recent progress CO2RR on MOF-based materials toward First, structure MOFs is briefly introduced. Then, performance corresponding catalytic mechanism pristine (classified according kind organic ligands/linkers) MOF-derived (including metal nanomaterials, single-atom catalysts nanocomposites) product systematically discussed. Finally, critical challenges opportunities highlighted inspire rational design targeted synthesis advanced high-performance

Язык: Английский

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Advanced Catalyst Design and Reactor Configuration Upgrade in Electrochemical Carbon Dioxide Conversion

Advanced Materials, Год журнала: 2023, Номер 35(52)

Опубликована: Авг. 20, 2023

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) driven by renewable energy shows great promise in mitigating and potentially reversing the devastating effects of anthropogenic climate change environmental degradation. The simultaneous synthesis energy‐dense chemicals can meet global demand while decoupling emissions from economic growth. However, development CO RR technology faces challenges catalyst discovery device optimization that hinder their industrial implementation. In this contribution, a comprehensive overview current state research is provided, starting with background motivation for technology, followed fundamentals evaluated metrics. Then underlying design principles electrocatalysts are discussed, emphasizing structure–performance correlations advanced electrochemical assembly cells increase selectivity throughput. Finally, review looks to future identifies opportunities innovation mechanism discovery, material screening strategies, assemblies move toward carbon‐neutral society.

Язык: Английский

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Ligand Design in Atomically Precise Copper Nanoclusters and Their Application in Electrocatalytic Reactions

Advanced Functional Materials, Год журнала: 2023, Номер 33(44)

Опубликована: Июль 2, 2023

Abstract Metal nanoclusters (MNCs) are compositionally well‐defined and also structurally precise materials with unique molecule‐like properties discrete electronic energy levels. Atomically ligand‐protected Cu (LP‐CuNCs) one category of typical MNCs that usually demonstrate geometric structures to serve as electrocatalysts. However, the synthesis, application, well structure‐performance relationship LP‐CuNCs not adequately studied. Significantly, ligands essential structure, crystal size, structure LP‐CuNCs, which determine their physiochemical applications. In this review, significant progress in ligand design application electrocatalytic reactions is introduced. The general basics (LP‐MNCs) first introduced functions emphasized. Subsequently, a series different for including thiolates, phosphines, alkynyl, polymers, biomolecules highlighted. Thereafter, applications discussed. It believed review will only inspire synthesis novel but contribute extension establishment accurate relationships.

Язык: Английский

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Acidic conditions for efficient carbon dioxide electroreduction in flow and MEA cells

Chem Catalysis, Год журнала: 2023, Номер 3(8), С. 100670 - 100670

Опубликована: Июнь 21, 2023

Язык: Английский

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