华中科技大学李箐团队报道了通过调节超薄Au₃Pt双纳米线上Au-Pt配位的自发产氢与葡萄糖增值。相关研究成果于2025年1月20日发表在国际顶尖学术期刊《德国应用化学》。

有机物电氧化耦合制氢因其低运行电压而受到越来越多的关注。然而，自发产生氢气并结合有机物稳定化仍然具有挑战性。

该文中，研究人员开发了超薄Au/Pt双纳米线（NW）催化剂，用于电化学葡萄糖氧化和自发制氢系统的析氢反应。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助于选择性葡萄糖电氧化为葡萄糖酸（GNA）（0.07 VRHE的低起始电位和>90%的选择性）。

原位光谱和理论计算表明，Au₃Pt-NWs可以通过“Pt到Au位点转移”机制降低GNA产生的能量势垒，减轻Pt位点的中毒，这有助于强吸收葡萄糖酸内酯的解吸。因此，配备Au₃Pt-NWs催化剂的不对称电池实现了自发氢气生产和葡萄糖稳定化，峰值功率为50 mW，在50 mA cm^-2下输出0.24 V的电压，优于最先进的氢气生产电解槽。该装置生产1公斤氢气的同时，阳极产品的价格为64.2美元（GNA为1200美元吨^-1），发电量为5.36千瓦时。

附：英文原文

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

Author: Hao Shi, Tanyuan Wang, Zijie Lin, Shuxia Liu, Xuan Liu, Ruixin Zhou, Zhao Cai, Yunhui Huang, Qing Li

Issue&Volume: 2025-01-20

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 NW 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.

DOI: 10.1002/anie.202424476

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202424476