Water adlayers bridging metal spillover to boost catalytic activity.

IF 15.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Yamei Fan,Rongtan Li,Xiangze Du,Fei Wang,Xiaohui Feng,Youyuanhe Yang,Conghui Liu,Jiaxin Li,Cui Dong,Jianyang Wang,Na Ta,Wenhao Cui,Yanxiao Ning,Rentao Mu,Qiang Fu
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引用次数: 0

Abstract

Hydrogen spillover has been extensively studied in heterogeneous catalysis, whereas the analogous migration of metal species remains largely underexplored. Here, we report a spillover phenomenon for metal species, exemplified by copper, which spontaneously migrates across physically contacted hydrophilic supports under humid ambient conditions. This process is facilitated by water adlayers on support surfaces, which act as molecular bridges to enable surface and interfacial migration of cooper species via hydroxylated intermediates. The phenomenon is universal across diverse supports, including oxides, carbides, and sulfides, and extends to metals such as ruthenium, cobalt, and nickel. Remarkably, catalysts prepared via this spillover approach exhibit substantially enhanced low-temperature activity in reactions including carbon monoxide oxidation, reverse water-gas shift, selective catalyst reduction with ammonia, and hydrogen cyanide oxidation, outperforming counterparts prepared by conventional impregnation. This work redefines the spillover phenomenon by extending it to metal species through water adlayer-mediated migration, opening new avenues for the design of dynamic catalysts.
水垫桥接金属溢出以提高催化活性。
氢外溢在多相催化中得到了广泛的研究,而金属物种的类似迁移仍未得到充分的探索。在这里,我们报告了金属物种的溢出现象,以铜为例,在潮湿的环境条件下,铜会自发地迁移到物理接触的亲水载体上。支撑表面的水层促进了这一过程,水层作为分子桥梁,通过羟基化中间体实现铜的表面和界面迁移。这种现象在不同的支撑物中是普遍存在的,包括氧化物、碳化物和硫化物,并延伸到钌、钴和镍等金属。值得注意的是,通过这种溢出方法制备的催化剂在一氧化碳氧化、逆水气转换、氨选择性催化剂还原和氰化氢氧化等反应中表现出显著增强的低温活性,优于传统浸渍方法制备的催化剂。这项工作重新定义了溢出现象,通过水层介导的迁移将其扩展到金属物种,为动态催化剂的设计开辟了新的途径。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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