Manipulating the Water Dissociation Electrocatalytic Sites of Bimetallic Nickel-Based Alloys for Highly Efficient Alkaline Hydrogen Evolution.

Angew Chem Int Ed Engl

Institute of Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, 325035, Wenzhou, Zhejiang, P. R. China.

Published: July 2022

Transition-metal alloys are currently drawing increasing attention as promising electrocatalysts for the alkaline hydrogen evolution reaction (HER). However, traditional density-functional-theory-derived d-band theory fails to describe the hydrogen adsorption energy (ΔG ) on hollow sites. Herein, by studying the ΔG for a series of Ni-M (M=Ti, V, Cr, Mn, Fe, Co, Cu, Zn, Mo, W) bimetallic alloys, an improved d-band center was provided and a potential NiCu electrocatalyst with a near-optimal ΔG was discovered. Moreover, oxygen atoms were introduced into Ni-M (O-NiM) to balance the adsorption/desorption of hydroxyl species. The tailored electrocatalytic sites for water dissociation can synergistically accelerate the multi-step alkaline HER. The prepared O-NiCu shows the optimum HER activity with a low overpotential of 23 mV at 10 mA cm . This work not only broadens the applicability of d-band theory, but also provides crucial understanding for designing efficient HER electrocatalysts.

Download full-text PDF

Source
http://dx.doi.org/10.1002/anie.202202518DOI Listing

Publication Analysis

Top Keywords

water dissociation
8
electrocatalytic sites
8
alkaline hydrogen
8
hydrogen evolution
8
d-band theory
8
manipulating water
4
dissociation electrocatalytic
4
sites bimetallic
4
bimetallic nickel-based
4
nickel-based alloys
4

Similar Publications

Drug Development.

Alzheimers Dement

December 2024

Yonsei University, Incheon, Incheon, Korea, Republic of (South).

Background: The accumulation of amyloidogenic proteins is recognized as a primary biomarker, initiator of pathology, and a potential therapeutic target for Alzheimer's disease (AD). An unbiased screening of a small molecule library was conducted to identify new chemical compounds exhibiting amyloid-dissociative properties.

Method: The ability of aryloxypropanolamine derivatives to dissociate amyloid-β (Aβ) aggregates was evaluated through in vitro assays.

View Article and Find Full Text PDF

In processes such as electrodialysis, the applied electrical potential is constrained by concentration polarization at the membrane/solution interface. This polarization, which intensifies at higher current densities, impedes ion transport efficiency and may lead to problems such as salt precipitation, membrane degradation, and increased energy consumption. Therefore, understanding concentration polarization is essential for enhancing membrane performance, improving efficiency, and reducing operational costs.

View Article and Find Full Text PDF

Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials.

Adv Mater

January 2025

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China.

Nitrate electroreduction is promising for achieving effluent waste-water treatment and ammonia production with respect to the global nitrogen balance. However, due to the impeded hydrogenation process, high overpotentials need to be surmounted during nitrate electroreduction, causing intensive energy consumption. Herein, a hydroxide regulation strategy is developed to optimize the interfacial HO behavior for accelerating the hydrogenation conversion of nitrate to ammonia at ultralow overpotentials.

View Article and Find Full Text PDF

Hydrogen-localization Transfer Regulation in 3D COFs Enhances Photocatalytic Acetylene Semi-hydrogenation to Ethylene.

Angew Chem Int Ed Engl

January 2025

South China Normal University, school of chemistry, No. 378, Waihuan West Road, Panyu District, 510006, Guangzhou, CHINA.

In this work, a series of new crystalline three-dimensional covalent organic frameworks (3D COFs) based on [8+4] construction was designed and successfully realized efficient photocatalytic acetylene (C2H2) hydrogenation to ethylene (C2H4). By regulating the hydrogen-localization transfer effect in these 3D COFs,the Cz-Co-COF-H containing cobalt glyoximate active centers exhibited excellent C2H2-to-C2H4 performance, with an average C2H4 yield of 1755.33 μmol g-1 h-1 in pure C2H2, also showed near 100% conversion of C2H2 in 1% C2H2 contained crude C2H4 mixtures (industry-relevant conditions), and finally obtain polymer grade C2H4.

View Article and Find Full Text PDF

Rational regulation of active hydrogen (*H) behavior is crucial for advancing electrocatalytic nitrate reduction reaction (NO3RR) to ammonia (NH3), yet in-depth understanding of the *H generation, transfer, and utilization remains ambiguous, and explorations for *H dynamic optimization are urgently needed. Herein we engineer a Ni3N nanosheet array intimately decorated with Cu nanoclusters (NF/Ni3N-Cu) for remarkably boosted NO3RR. From comprehensive experimental and theoretical investigations, the Ni3N moieties favors water dissociation to generate *H, and then *H can rapidly transfer to the Cu via unique reverse hydrogen spillover mediating interfacial Ni-N-Cu bridge bond, thus increasing *H coverage on the Cu site for subsequent deoxygenation/hydrogenation.

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!