Direct Synthesis of Pure Aqueous H2O2 Solution within Aluminosilicate Zeolite Crystals
Direct Synthesis of Pure Aqueous H2O2 Solution within Aluminosilicate Zeolite Crystals
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DOI：
10.1021/acscatal.0c05103
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发表时间：
2021-01-29
期刊：
影响因子：
12.9
通讯作者：
Xiao, Feng-Shou
中科院分区：
文献类型：
--
作者：
Jin, Zhu;Liu, Yifeng;Xiao, Feng-Shou
过氧化氢的合成一般需要多种混合有机溶剂和/或卤化物添加剂，导致提纯复杂。在这里，我们克服了这个问题，通过使用固定在铝硅酸盐沸石晶体中的AuPd纳米粒子作为催化剂，在水溶液中直接合成过氧化氢。AuPd纳米粒子通过分子筛辅助的质子转移过程催化分子筛晶体中的氧加氢生成过氧化氢。此外，质子还稳定了过氧化氢产物，防止了导致过氧化氢分解的去质子化。在水中，H_2O_2的产率达到320 mmolg(AuPd)(-1)h~(-1)，H-2选择性为88%，与传统负载型金属纳米粒子催化剂相比有了很大的进步。这些发现突出了沸石的固定结构，为设计高效的H_2O_2合成催化剂提供了新的途径。
The synthesis of H2O2 generally requires multiple mixed organic solvents and/or halide additives, causing complexity in purification. Herein, we overcome this problem by direct synthesis of H2O2 in aqueous solution using AuPd nanoparticles fixed within the aluminosilicate zeolite crystals as a catalyst. The AuPd nanoparticles catalyzed the oxygen hydrogenation to form H2O2 in zeolite crystals via a zeolite-assisted proton transfer process. In addition, the protons also stabilize the H2O2 product against the deprotonation that causes H2O2 decomposition. The H2O2 productivity reached 320 mmol g(AuPd)(-1) h(-1) with a H-2 selectivity of 88% in water, showing significant advances compared with the conventionally supported metal nanoparticle catalysts. These findings highlight the zeolite fixed structure that offers a new way for designing efficient catalysts in H2O2 synthesis.