Optimizing Intermediate Adsorption via Heteroatom Ensemble Effect over RuFe Bimetallic Alloy for Enhanced Nitrate Electroreduction to Ammonia

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(31)

Published: June 30, 2023

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach for removal and NH synthesis at ambient conditions. As complex eight‐electron/nine‐proton transfer process, its performance relies heavily on the adsorption ability of intermediates catalyst surface, which determined by geometric electronic configurations active sites. In this work, heteroatom ensemble effect deliberately triggered over RuFe bimetallic alloy to optimize intermediate NO RR. A record‐high yield rate 118.8 mg h −1 high Faradaic efficiency 92.2% are achieved −1.4 V vs reversible hydrogen electrode, ranking top state‐of‐the‐art. Experimental computational results reveal that characteristics induced play crucial roles. Both Ru Fe display continuous state throughout Fermi level, suggesting electron density benefits whole result, facilitated − , efficient stabilization key intermediates, as well timely desorption simultaneously achieved, thus significantly promoting direct .

Language: Английский

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Comprehensive understanding of the thriving electrocatalytic nitrate/nitrite reduction to ammonia under ambient conditions

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 92, P. 459 - 483

Published: Jan. 4, 2024

Language: Английский

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Achieving Near 100% Faradaic Efficiency of Electrocatalytic Nitrate Reduction to Ammonia on Symmetry-Broken Medium-Entropy-Alloy Metallene

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(10), P. 7907 - 7916

Published: May 6, 2024

Electrochemical nitrate reduction (NO3RR) offers an ecofriendly way for ammonia production. However, improving the sluggish kinetics of such a multistep reaction still remains challenging. Herein, asymmetry strategy is proposed to adjust charge distribution active centers on metallene by presenting novel symmetry-broken medium-entropy-alloy (MEA) via heteroatom alloying. Benefiting from maximized exposure well-regulated sites, proof-of-concept PdCuCo MEA delivers near 100% NH3 Faradaic efficiency in both neutral and alkaline electrolytes, along with record-high yield rate over 532.5 mg h–1 mgcat–1. Moreover, it enables 99.7% conversion industrial wastewater level 6200 ppm drinkable water level. Detailed studies further revealed that redistribution induced elemental electronegativity difference metallene, which will weaken N–O bond *NO, thus reducing energy barrier rate-determining step. Meanwhile, competitive HER formation NO2– are also hindered. We believe our this work shed light design efficient NO3RR catalysts more practical

Language: Английский

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Bio-inspired designs for wet gas sensing systems and beyond

Device, Journal Year: 2024, Volume and Issue: 2(3), P. 100293 - 100293

Published: March 1, 2024

Language: Английский

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Identifying Upper d-Band Edge as Activity Descriptor for Ammonia Oxidation on PtCo Alloys in Low-Temperature Direct Ammonia Fuel Cells

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 3, 2025

Low-temperature direct ammonia fuel cell (DAFC) stands out as a more secure technology than the hydrogen system, while there is still lack of elegant bottom-up synthesis procedures for efficient oxidation reaction (AOR) electrocatalysts. The widely accepted d-band center, even with consideration width, usually fails to describe variations in AOR reactivity many practical conditions, and accurate activity descriptor necessary less empirical path. Herein, upper edge, εu, derived from model, identified an effective accurately establishing descriptor–activity relationship. Using PtCo alloy varying atomic composition example, εu value succeeds reflecting corresponding trends activity, showing striking linear correlation coefficient determination (R2) high 0.90. effectiveness established relationship verified experimentally. optimum electrocatalyst delivers excellent peak current density 74.04 A g–1 at 5 mV s–1, assembled DAFC generates power density, outperforming majority extensively reported systems. This work brings fundamental insights into between chemical electronic structure benefits rational optimization next-generation low-temperature DAFC.

Language: Английский

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Research Progress of Coordination Materials for Electrocatalytic Nitrogen Oxides Species Conversion into High-Value Chemicals

EnergyChem, Journal Year: 2025, Volume and Issue: unknown, P. 100146 - 100146

Published: Feb. 1, 2025

Language: Английский

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Next Generation Noble Metal‐Engineered Catalysts: From Structure Evolution to Structure‐Reactivity Correlation in Water Splitting

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(4)

Published: Oct. 20, 2023

Abstract Noble metal‐engineered catalysts (NMECs) play an important role in promoting the practical utilization of water‐splitting devices hydrogen energy systems. While owing to complicated catalytic centers, diverse support structures, and changing microenvironments, NMECs still face many challenges when it comes designing analyzing precise sites activity‐mechanism analyses, which are crucial for their future developments. Here, this cutting‐edge review systematically discusses recent advancements water electrolysis, including structure evolution, microenvironment modulation, structure‐reactivity correlation, new horizons. First, fundamental advantages, mechanisms, evaluation methods splitting outlined. Then, strategies modulate microenvironments thoroughly summarized, such as crystal phase alloying effects, crystallization degrees, size substrate effects. In particular, there valuable perspectives on bond interactions, theoretical calculations, disclose mechanisms. Thereafter, a special emphasis is given performances, devices. Finally, thorough discussion upcoming difficulties directions developing next‐generation presented. It believed that will have significant influence creating noble metal‐based field electrolytic water‐splitting.

Language: Английский

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Recent Advances in Electrocatalysts for Sustainable Electrosynthesis of Ammonia and Urea from Ambient Nitrite Reduction and C–N Coupling

ACS Materials Letters, Journal Year: 2023, Volume and Issue: 5(12), P. 3347 - 3363

Published: Nov. 21, 2023

The global nitrogen cycle has been destroyed by the quickly growing anthropogenic emissions of nitrite-containing pollutants during past decades, which causes numerous unexpected environmental side effects and threatens human health. Compared with conventional nitrite removal methods featuring low efficiency, high cost, secondary pollution, electrocatalytic reduction reaction garnered significant attention offers an appealing solution for recovering balance. Moreover, it takes a step further to convert into recyclable nitrogen-containing fertilizer including ammonia urea. However, materials design mechanistic aspects such emerging complex reactions are yet be explored compared other well-studied primary as oxygen water splitting. To address this challenge, review provides comprehensive account sustainable electrosynthesis urea from ambient C–N coupling. two key reactions, namely production synthesis coreduction carbon dioxide, elaborated in detail, available catalysts focus discussion. current technical barriers potential research prospects domain, exploring excellent electrocatalysts activity selectivity, precisely controlling interfacial microenvironment, understanding in-depth mechanism, highlighted.

Language: Английский

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Interfacial Proton Supply/Filtration Regulates the Dynamics of Electrocatalytic Nitrogen Reduction Reaction: A Perspective

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(44)

Published: July 6, 2023

Abstract As a promising energy carrier, ammonia synthesis by electrocatalytic nitrogen reduction reaction (eNRR) is green and low‐carbon strategy that can replace the traditional Haber–Bosch process. However, development of eNRR processes mainly severely constrained competitive hydrogen evolution (HER), corresponding strategies to inhibit this adverse side obtain high selectivity are still limited. In addition, for complex involving gas–liquid–solid three‐phase interface proton/electron transfer, it great significance analyze summarize existing inhibition HER from viewpoint dynamics. view this, work reviews proton supply/filtration regulation in catalytic system, allowing systematic survey literature focusing on membrane (inorganic organic membrane), electrolyte (metal‐mediated ion strategy) system device design (electrode structure electrolytic cell design). Constructive guidance also suggested improve NH 3 selectivity, aiming scalable economically feasible applications.

Language: Английский

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Acid oxygen evolution reaction: Mechanisms, design principles, and prospects for application in membrane electrodes

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: unknown, P. 155901 - 155901

Published: Sept. 1, 2024

Language: Английский

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