Developing efficient oxygen evolution reaction (OER) electrocatalysts is important for enhancing the water splitting efficiency. However, with the current catalysts containing one kind of active sites, it is challenging to achieve low overpotentials because of the four-electron transfer process. Herein is reported HZIF-2-CoMo, a new metal-organic framework with well-defined Co-Mo dual sites that can promote the OER process through an unconventional Mo/Co dual-site relay mechanism. Theoretical calculations suggested that the Mo and Co sites stabilize the HO* and HOO* intermediates, respectively, and that the unique Co-O-Mo configuration induces the formation of a Co-O*-Mo transition intermediate, remarkably reducing the reaction free energy. As a result, HZIF-2-CoMo shows an overpotential of 277 mV at 10 mA cm and a low Tafel slope of 70 mV dec in alkaline solution, making it one of the best OER electrocatalysts reported to date.
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http://dx.doi.org/10.1021/acs.inorgchem.0c03359 | DOI Listing |
ACS Appl Mater Interfaces
January 2025
Energy and Process Engineering Division, School of Mechanical, Medical and Process Engineering, Science and Engineering Faculty, Queensland University of Technology, 2 George Street, Brisbane City, Queensland 4001, Australia.
The strategic design and fabrication of efficient electrocatalysts are pivotal for advancing the field of electrochemical water splitting (EWS). To enhance EWS performance, integrating non-noble transition metal catalysts through a cooperative double metal incorporation strategy is important and offers a compelling alternative to conventional precious metal-based materials. This study introduces a novel, straightforward, single-step process for fabricating a bimetallic MoCo catalyst integrated within a three-dimensional (3D) nanoporous network of N, P-doped carbon nitride derived from a self-contained precursor.
View Article and Find Full Text PDFJ Hazard Mater
December 2024
Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650050, PR China; Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming 650500, PR China; Key Laboratory of Yunnan Province for Synthesizing Sulfur-containing Fine Chemicals, The Innovation Team for Volatile Organic Compounds Pollutants Control and Resource Utilization of Yunnan Province, The Higher Educational Key Laboratory for Odorous Volatile Organic Compounds Pollutants Control of Yunnan Province, Kunming 650500, PR China. Electronic address:
The catalytic degradation of malodorous sulfur-containing volatile organic compounds (S-VOCs), especially methanethiol (CHSH), faces an enormous challenge in striking a balance between activity and stability. Herein, we develop the time-tandem and spatial-extended strategy for synthesizing t-MoO/meso-SiO nano-reactor-type catalysts and reveal the migration and transformation behaviors of both carbon and sulfur species at the mesoscopic scale to break the catalytic CHSH activity and stability trade-off. The dynamic evolution of active centers from initial oxygen sites and acid sites to sulfur vacancies in MoS during the reaction process as well as the formation of a new dimethyl disulfide (CHSSCH) reaction pathway are identified as the main reason for the catalysts' superior activity and sulfur resistance.
View Article and Find Full Text PDFJ Colloid Interface Sci
January 2025
College of Energy Engineering, Huanghuai University, Zhumadian 463000, China. Electronic address:
Herein, a novel liquid nitrogen quenching treatment is proposed to achieve multifaceted modulation involving morphological modulation, lattice tensile strain modulation, metal active centre coordination reconstruction and grain boundary construction within a series of intermetallic compounds modified on a carbon substrate (CoFe-550/C, CoNi-550/C and FeNi-550/C, where 550 refers to liquid nitrogen quenching temperature and C refers to the carbon substrate). Noteworthily, the optimising intermediate absorption/desorption process is achieved by multifaceted modulation. Consequently, CoFe-550/C, CoNi-550/C and FeNi-550/C demonstrate considerable overpotential for hydrogen evolution reaction (59.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea.
Iridium single atom catalysts are promising oxygen evolution reaction (OER) electrocatalysts for proton exchange membrane water electrolysis (PEMWE), as they can reduce the reliance on costly Ir in the OER catalysts. However, their practical application is hindered by their limited stability during PEMWE operation. Herein, we report on the activation of Ir-doped CoMnO in acidic electrolyte that leads to enhanced activity and stability in acidic OER for long-term PEMWE operation.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
School of Chemistry, Beijing Advanced Innovation Center for Biomedical Engineering, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology, Beihang University, Beijing 100191, China.
The dual-site synergistic catalytic mechanism on NiFeOOH suggests weak adsorption of Ni sites and strong adsorption of Fe sites limited its activity toward alkaline oxygen evolution reaction (OER). Large-scale density functional theory (DFT) calculations confirm that Co doping can increase Ni adsorption, while the metal vacancy can reduce Fe adsorption. The combined two factors can further modulate the atomic environment and optimize the free energy toward oxygen-containing intermediates, thus enhancing the OER activity.
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