The rational design of highly efficient and stable electrocatalysts for the oxygen evolution reaction (OER) is an urgent need but remains challenging for various sustainable energy systems. How to adjust the atomic structure and electronic structure of the active center is a key bottleneck problem. Accelerating the electron transfer process and the deep self-reconstruction of active sites could be a cost-effective strategy toward electrocatalytic OER catalyst development. Here, a crystalline-amorphous (c-a) coupled NiS/NiP electrocatalyst self-supported on nickel foam with an intimate interface was developed via a feasible solvothermal-electrochemistry method. The coupling interface of the crystalline structure with high conductivity and amorphous structure with numerous potential active sites could regulate the electronic structure and optimize the adsorption/desorption of O-containing species, ultimately resulting in high OER catalytic performance. The obtained NiS/NiP/NF presents a low OER overpotential of 265 mV to obtain 10 mA·cm and a small Tafel slope of 51.6 mV·dec. Also, the catalyst with the coupled interface exhibited significantly enhanced long-term stability compared to the other two catalysts, with <5% decay in OER activity over 20 h of continuous operation, while that of NiS/NF and NiP/NF decreased by about 30 and 50%, respectively. This study provides inspiration for other energy conversion reactions in optimizing the performance of catalysts by coupling crystalline-amorphous structures.
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http://dx.doi.org/10.1021/acsami.3c00547 | DOI Listing |
Chem Rev
January 2025
Department of Chemical & Biomolecular Engineering, University of California, Irvine, California 92697, United States.
The reactions critical for the energy transition center on the chemistry of hydrogen, oxygen, carbon, and the heterogeneous catalyst surfaces that make up electrochemical energy conversion systems. Together, the surface-adsorbate interactions constitute the electrochemical interphase and define reaction kinetics of many clean energy technologies. Practical devices introduce high levels of complexity where surface roughness, structure, composition, and morphology combine with electrolyte, pH, diffusion, and system level limitations to challenge our ability to deconvolute underlying phenomena.
View Article and Find Full Text PDFNano Lett
January 2025
Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea.
Solar-powered electrochemical NH synthesis offers the benefits of sustainability and absence of CO emissions but suffers from a poor solar-to-ammonia yield rate (SAY) due to a low NH selectivity, large bias caused by the sluggish oxygen evolution reaction, and low photocurrent in the corresponding photovoltaics. Herein, a highly efficient photovoltaic-electrocatalytic system enabling high-rate solar-driven NH synthesis was developed. A high-performance Ru-doped Co nanotube catalyst was used to selectively promote the nitrite reduction reaction (NORR), exhibiting a faradaic efficiency of 99.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Northeast Forestry University, Chemical Engineering and Resource Utilization, CHINA.
Electrochemical 5-hydroxymethylfurfural (HMF) oxidation reaction (HMFOR) offers a promising route to transform biomass into value-added chemicals. However, the competing oxygen evolution reaction (OER) greatly limits the HMFOR selectivity. Herein, we report a facile doping strategy to engineer oxygen intermediates adsorption on amorphous NiFe alloys to boost highly selective electrochemical HMF oxidation to produce 2,5-furandicarboxylic acid (FDCA), among which, amorphous Mn-doped NiFeB alloy displays a low HMFOR onset potential of 1.
View Article and Find Full Text PDFAdv Mater
January 2025
Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
The safety of the P2-type layered transition metal oxides (P2-NaTMO), a promising cathode material for sodium-ion batteries (SIBs), is a prerequisite for grid-scale energy storage systems. However, previous thermal runaway studies mainly focused on morphological changes resulting from gas production detection and thermogravimetric analysis, while the structural transition and chemical reactions underlying these processes are still unclear. Herein, a comprehensive methodology to unveil an interplay mechanism among phase structures, interfacial microcrack, and thermal stability of the charged P2-NaNiMnO (NNMO) and the P2-NaNiLiMnO (NNMO-Li) at elevated temperatures is established.
View Article and Find Full Text PDFAdv Mater
January 2025
School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore.
Developing highly efficient catalysts to accelerate sluggish electrode reactions is critical for the deployment of sustainable aqueous electrochemical technologies, yet remains a great challenge. Rationally integrating functional components to tailor surface adsorption behaviors and adsorbate dynamics would divert reaction pathways and alleviate energy barriers, eliminating conventional thermodynamic constraints and ultimately optimizing energy flow within electrochemical systems. This approach has, therefore, garnered significant interest, presenting substantial potential for developing highly efficient catalysts that simultaneously enhance activity, selectivity, and stability.
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