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1.
Proc Natl Acad Sci U S A ; 121(30): e2405846121, 2024 Jul 23.
Artigo em Inglês | MEDLINE | ID: mdl-39012829

RESUMO

High-entropy compounds have been emerging as promising candidates for electrolysis, yet their controllable electrosynthesis strategy remains a formidable challenge because of the ambiguous ionic interaction and codeposition mechanism. Herein, we report a oxygenates directionally induced electrodeposition strategy to construct high-entropy materials with amorphous features, on which the structural evolution from high-entropy phosphide to oxide is confirmed by introducing vanadate, thus realizing the simultaneous optimization of composition and structure. The representative P-CoNiMnWVOx shows excellent bifunctional catalytic performance toward alkaline hydrogen evolution reaction and ethanol oxidation reaction (EOR), with small potentials of -168 mV and 1.38 V at 100 mA cm-2, respectively. In situ spectroscopy illustrates that the electrochemical reconstruction of P-CoNiMnWVOx induces abundant Co-O species as the main catalytic active species for EOR and follows the conversion pathway of the C2 product. Theoretical calculations reveal the optimized electronic structure and adsorption free energy of reaction intermediates on P-CoNiMnWVOx, thereby resulting in a facilitated kinetic process. A membrane-free electrolyzer delivers both high Faradaic efficiencies of acetate and H2 over 95% and superior stability at100 mA cm-2 during 120 h electrolysis. In addition, the unique composition and structural advantages endow P-CoNiMnWVOx with multifunctional catalytic activity and realize multipathway electrosynthesis of formate-coupled hydrogen production.

2.
J Colloid Interface Sci ; 676: 13-21, 2024 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-39018806

RESUMO

Coupling hydrazine oxidation reaction (HzOR) with hydrogen evolution reaction (HER) has been widely concerned for high efficiency of green hydrogen preparation with low energy consumption. However, the lacking of bifunctional electrodes with ampere-level performance severely limits its industrialization. Herein, we put forward an efficient active site anchored strategy for MnCo2O4 nanosheet arrays on nickel foam (NF) by introducing Pt species (denoted as Pt-MnCo2O4/NF), which is standing for excellent bifunctional electrodes. The Pt-MnCo2O4/NF delivers ultralow potentials of -195 mV and 350 mV at 1000 mA cm-2 as well as robust stability for HzOR and HER, respectively. The study of in-situ Raman and reaction kinetics reveal that the formation of key adsorbed *NH2 and *N2H4 intermediates and the rapidly oxidization of intermediates with a fast interfacial charge transfer on Pt-MnCo2O4/NF. Remarkably, the Pt-MnCo2O4/NF assembled two-electrode hydrazine assisted water electrolyzer realizes current density of 100 mA cm-2 and 1000 mA cm-2 at 0.16 V and 0.62 V with over 80 h stability. This work provides a promising way to design efficient electrodes for energy-saving H2 generation under ampere-level current density.

3.
Dalton Trans ; 52(36): 12733-12741, 2023 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-37610334

RESUMO

The exploitation of high-performance electrocatalysts to achieve the economic electrocatalytic hydrogen evolution reaction (HER) is significant in generating H2 fuel. Enhancing the activity of the carrier catalyst by modifying trace precious metals is one of the important strategies. Herein, a hybrid material is developed by incorporating trace Ru species into a bimetallic phosphide (NiCoP) matrix on nickel foam (NF), showing a superior catalytic activity for HER. The Ru-NiCoP/NF hybrid material has plenty of heterointerfaces, improved electronic interaction, and small interfacial charge transfer resistance, improving the reaction kinetics of the HER. Remarkable, the Ru-NiCoP/NF provides a low overpotential of 96 mV at the current density of 50 mA cm-2 and high stability in 1.0 M KOH solution presenting a promising potential for hydrogen production. In addition, the Ru-NiCoP/NF sample exhibits the highest TOF value of 0.54 s-1 at an overpotential of 100 mV, which outperforms the commercial Ru/C catalyst. This study offers a promising approach for the synthesis of other precious metal supported hybrid materials.

4.
J Inequal Appl ; 2018(1): 268, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30363771

RESUMO

In this paper, we introduce a family of G B S operators of bivariate tensor product of λ-Bernstein-Kantorovich type. We estimate the rate of convergence of such operators for B-continuous and B-differentiable functions by using the mixed modulus of smoothness, establish the Voronovskaja type asymptotic formula for the bivariate λ-Bernstein-Kantorovich operators, as well as give some examples and their graphs to show the effect of convergence.

5.
J Inequal Appl ; 2018(1): 61, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-29576718

RESUMO

In this paper, we introduce a new type λ-Bernstein operators with parameter [Formula: see text], we investigate a Korovkin type approximation theorem, establish a local approximation theorem, give a convergence theorem for the Lipschitz continuous functions, we also obtain a Voronovskaja-type asymptotic formula. Finally, we give some graphs and numerical examples to show the convergence of [Formula: see text] to [Formula: see text], and we see that in some cases the errors are smaller than [Formula: see text] to f.

6.
J Inequal Appl ; 2017(1): 284, 2017.
Artigo em Inglês | MEDLINE | ID: mdl-29213195

RESUMO

In this paper, we construct a bivariate tensor product generalization of Kantorovich-type Bernstein-Stancu-Schurer operators based on the concept of [Formula: see text]-integers. We obtain moments and central moments of these operators, give the rate of convergence by using the complete modulus of continuity for the bivariate case and estimate a convergence theorem for the Lipschitz continuous functions. We also give some graphs and numerical examples to illustrate the convergence properties of these operators to certain functions.

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