Triggering Water and Methanol Activation for Solar-Driven H2 Production: Interplay of Dual Active Sites over Plasmonic ZnCu Alloy
Triggering Water and Methanol Activation for Solar-Driven H2 Production: Interplay of Dual Active Sites over Plasmonic ZnCu Alloy
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触发水和甲醇活化以进行太阳能驱动的 H-2 生产：等离激元 ZnCu 合金上双活性位点的相互作用
DOI：
10.1021/jacs.1c04315
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发表时间：
2021-07-29
影响因子：
15
通讯作者：
Ye, Jinhua
中科院分区：
文献类型：
--
作者：
Luo, Shunqin;Lin, Huiwen;Ye, Jinhua
甲醇水蒸气重整（MSR）是一种很有前途的反应，可以有效地生产和安全地运输氢气，但它需要相对较高的温度来实现高活性，导致大量的能量消耗。在这里，我们报告了一种等离子体ZnCu合金催化剂，由表面沉积Zn原子的等离子体Cu纳米颗粒组成，用于高效的太阳能驱动的MSR，而无需额外的热能输入。实验结果和理论计算表明，锌原子不仅作为水还原的催化位点，具有较低的活化能，但也作为电荷转移通道，泵热电子到水分子，随后导致形成缺电子铜甲醇活化。这些优点与光热加热一起使得最佳ZnCu催化剂在7.9 Suns照射下具有328 mmol gcatalytic（-1）h（-1）的高H-2产率和1.2%的太阳能转换效率，远远超过了已报道的常规光催化和热催化MSR。这项工作提供了一个潜在的策略，高效的太阳能驱动的氢气生产和其他各种能源需求的工业反应，通过设计合金催化剂。
Methanol steam reforming (MSR) is a promising reaction that enables efficient production and safe transportation of hydrogen, but it requires a relatively high temperature to achieve high activity, leading to large energy consumption. Here, we report a plasmonic ZnCu alloy catalyst, consisting of plasmonic Cu nanoparticles with surface-deposited Zn atoms, for efficient solar-driven MSR without additional thermal energy input. Experimental results and theoretical calculations suggest that Zn atoms act not only as the catalytic sites for water reduction with lower activation energy but also as the charge transfer channel, pumping hot electrons into water molecules and subsequently resulting in the formation of electron-deficient Cu for methanol activation. These merits together with photothermal heating render the optimal ZnCu catalyst a high H-2 production rate of 328 mmol gcatalyst(-1) h(-1) with a solar energy conversion efficiency of 1.2% under 7.9 Suns irradiation, far exceeding the reported conventional photocatalytic and thermocatalytic MSR. This work provides a potential strategy for efficient solar-driven H2 production and various other energy-demanding industrial reactions through designing alloy catalysts.