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铌酸作为硼氢化钠在温和条件下水解的微多相纳米催化的载体。

Niobic acid as a support for microheterogeneous nanocatalysis of sodium borohydride hydrolysis under mild conditions.

作者信息

Bousada Guilherme Mateus, Nogueira da Silva Victor, Fernandes de Souza Bárbara, de Oliveira Rodrigo Silva, Machado Junior Iterlandes, da Cunha Carlos Henrique Furtado, Astruc Didier, Teixeira Robson Ricardo, Lopes Moreira Renata Pereira

机构信息

Department of Chemistry, Universidade Federal de Viçosa Viçosa Minas Gerais 36570-000 Brazil

Institut des Sciences Moléculaires, Université de Bordeaux, UMR CNRS 5255 Talence 33405 Cedex France.

出版信息

RSC Adv. 2024 Jun 17;14(27):19459-19471. doi: 10.1039/d4ra01879f. eCollection 2024 Jun 12.

Abstract

This study explores the stabilization by niobic acid, of Pt, Ni, Pd, and Au nanoparticles (NPs) for the efficient microheterogeneous catalysis of NaBH hydrolysis for hydrogen production. Niobic acid is the most widely studied NbO polymorph, and it is employed here for the first time for this key reaction relevant to green energy. Structural insights from XRD, Raman, and FTIR spectroscopies, combined with hydrogen production data, reveal the role of niobic acid's Brønsted acidity in its catalytic activity. The supported NPs showed significantly higher efficiency than the non-supported counterparts regarding turnover frequency, average hydrogen production rate, and cost. Among the tested NPs, PtNPs and NiNPs demonstrate the most favorable results. The data imply mechanism changes during the reaction, and the kinetic isotope assay indicates a primary isotope effect. Reusability assays demonstrate consistent yields over five cycles for PtNPs, although catalytic efficiency decreases, likely due to the formation of reaction byproducts.

摘要

本研究探索了铌酸对铂、镍、钯和金纳米颗粒(NPs)的稳定作用,以实现硼氢化钠水解制氢的高效微多相催化。铌酸是研究最广泛的NbO多晶型物,首次用于这一与绿色能源相关的关键反应。X射线衍射(XRD)、拉曼光谱和傅里叶变换红外光谱(FTIR)的结构分析结果,结合产氢数据,揭示了铌酸的布朗斯台德酸度在其催化活性中的作用。负载型纳米颗粒在周转频率、平均产氢速率和成本方面表现出比非负载型纳米颗粒更高的效率。在测试的纳米颗粒中,铂纳米颗粒(PtNPs)和镍纳米颗粒(NiNPs)显示出最有利的结果。数据表明反应过程中机理发生了变化,动力学同位素分析表明存在一级同位素效应。可重复使用性测试表明,尽管催化效率下降,可能是由于反应副产物的形成,但PtNPs在五个循环中的产率保持一致。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9cc1/11182415/3c11dff1d73d/d4ra01879f-f1.jpg

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