Spontaneous Hydrogen Production Coupled with Glucose Valorization through Modulating Au-Pt Coordination on Ultrathin Au3Pt Twin Nanowires

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-01-20 DOI:10.1002/anie.202424476
Hao Shi, Prof. Tanyuan Wang, Zijie Lin, Shuxia Liu, Xuan Liu, Ruixin Zhou, Prof. Zhao Cai, Prof. Yunhui Huang, Prof. Qing Li
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Abstract

Organics electrooxidation coupled hydrogen production has attracted increasing attention due to the low operation voltage. Nevertheless, the spontaneous production of hydrogen coupled with organics valorization remains challenging. Herein, we develop ultrathin Au/Pt twin nanowire (NW) catalysts for both electrochemical glucose oxidation and hydrogen evolution reaction towards a spontaneous hydrogen production system. The more Pt−Au coordination and the localized tensile strain generated on twin boundaries of Au3Pt NWs facilitate the selective glucose electro-oxidation to gluconic acid (GNA) compared to Pt NWs (a low onset potential of 0.07 VRHE and selectivity >90 %). In situ spectroscopy and theoretical calculations reveal that Au3Pt NWs could reduce the energy barriers for GNA generation and alleviate the poisoning of Pt sites via a ′Pt-to-Au site transfer′ mechanism, which facilitates the desorption of strongly absorbed gluconolactone. Therefore, the asymmetric cell equipped with Au3Pt NWs catalysts realizes the spontaneous hydrogen production and glucose valorization with a peak power of 50 mW, which outputs the voltage of 0.24 V at 50 mA cm−2, outperforming the state-of-the-art electrolyzers for hydrogen production. The production of 1 kg H2 of the device is accompanied with $64.2 valorization of the anode product ($1200 ton−1 for GNA), and 5.36 kW h of generated electricity.

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通过调节超薄Au3Pt双纳米线上Au-Pt配位的自发产氢与葡萄糖增值
有机物电氧化偶联制氢因其工作电压低而受到越来越多的关注。然而,氢的自发生产与有机增值耦合仍然具有挑战性。在此,我们开发了超薄Au/Pt双纳米线(NW)催化剂,用于电化学葡萄糖氧化和自发产氢反应。与Pt NWs相比,更多的Pt- au配位和在Au3Pt NWs的孪晶界上产生的局部拉伸应变有利于选择性葡萄糖电氧化成葡萄糖酸(GNA) (0.07 VRHE的低电位和选择性>;90%)。原位光谱和理论计算表明,Au3Pt NWs可以降低GNA生成的能垒,并通过“Pt-to- au位点转移”机制减轻Pt位点的中毒,从而促进强吸收葡萄糖内酯的解吸。因此,配备了Au3Pt NW催化剂的不对称电解槽实现了自发制氢和葡萄糖增值,峰值功率为50 mW,输出电压为0.24 V,电压为50 mA cm-2,优于目前最先进的制氢电解槽。该装置生产1千克氢气,伴随着阳极产品的64.2美元增值(GNA为1200美元)和5.36千瓦时的发电量。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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