Surface reconstruction for efficient total hydrolysis

Surface reconstruction for efficient total hydrolysis
The rational construction of amorphous heterogeneous interfaces can effectively improve the activity and stability of hydrogen-extraction reaction (HER) and oxygen-extraction reaction (OER). In this paper, RuO2/Co3O4 (RCO) amorphous heterogeneous interfaces were prepared by oxidation method. The very good RCO-10 showed HER overpotentials of 57 and 231 mV, and an OER overpotential of 10 mA cm-2. Experimental characterization and density-functional theory (DFT) results showed that the optimized electronic structure and surface reconstruction resulted in the excellent catalytic activity of RCO-10.The DFT results indicated that the electron transfer from RuO2 to Co3O4, electron redistribution was achieved, which shifted the d-band center upward and optimized the adsorption free energy of the hydrogen reaction intermediates. In addition, the reconfigured Ru/Co(OH)2 has a lower hydrogen adsorption free energy in the HER process, which improves the HER activity. The reconstituted RuO2/CoOOH has a lower radical reaction energy barrier (O*→*OOH) in the OER process, which improves the OER activity. Moreover, RCO-10 required only 1.50 V to drive 10 mA cm-2 and remained stable for 200 h for total hydrolysis. Meanwhile, RCO-10 exhibited a stability of 48 h in an alkaline solution of 0.5 M NaCl. The amorphous heterogeneous interface may bring a new breakthrough in the design of efficient stabilized catalysts.


In summary, a facile oxidation method for the preparation of RuO2/Co3O4 (RCO) catalysts with amorphous heterogeneous interfaces is proposed in this paper. Unlike catalysts with crystal-crystal heterogeneous interfaces, this unique amorphous heterogeneous interface has a more flexible electronic structure and abundant defects, which can significantly optimize the electrocatalytic performance of the catalyst. As a result, the very best RCO-10 is characterized by a low overpotential and high stability of hydrogen-extraction reaction (HER) and oxygen-extraction reaction (OER) compared to other catalysts.RCO-10 requires only 1.50 V to drive 10 mA cm-2 for total hydrolysis. This excellent catalytic performance is attributed to the optimized electronic structure and surface reconstruction. This work provides a promising strategy for the preparation of other high-performance transition metal oxide catalysts with amorphous heterogeneous interfaces for efficient total hydrolysis.


Atomic-scale interfacial catalysts are those catalysts where the active components are dispersed or interact at the interface on an atomic scale in a catalytic reaction. The main objective of the design and utilization of such catalysts is to maximize the catalytic activity, improve the catalytic efficiency, and reduce the reaction activation energy to achieve a more efficient and environmentally friendly chemical reaction process.
In atomic-scale interfacial catalysts, the active components usually exist as individual atoms or very small clusters on the surface or at the interface of the catalyst. This high degree of dispersion allows the catalyst to have a very high atom utilization rate, which can greatly improve the catalytic activity. At the same time, the design of atomic-scale interfacial catalysts can also regulate the electronic structure and surface properties of the catalysts, thus optimizing the catalytic performance.


The preparation of atomic-scale interfacial catalysts usually requires the use of advanced nanotechnology and surface science tools, such as atomic layer deposition (ALD) and molecular beam epitaxy (MBE). These techniques allow precise control of the composition, structure and morphology of the catalysts, thus enabling atomic-scale design and modulation.
Atomic-scale interfacial catalysts have a wide range of applications in the fields of energy conversion and storage, environmental treatment, and organic synthesis. For example, in the fields of fuel cells and electrolytic hydrogen production, atomic-scale interfacial catalysts can improve the rate and efficiency of hydrogen generation and reduce energy consumption and cost; in environmental governance, atomic-scale interfacial catalysts can be used for efficient degradation of organic pollutants and catalytic conversion of greenhouse gases.
Overall, atomic level interfacial catalysts are a new type of efficient and environmentally friendly catalysts with broad application prospects and important scientific value. With the continuous development of nanotechnology and surface science, the design and preparation of atomic-level interfacial catalysts will be more precise and efficient, providing strong support for the realization of a green and sustainable chemical industry (Source: Nanostructured Materials).

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