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低原子序数钌原子簇辅助 III 族氮化物纳米线的氮光固定。

Nitrogen Photofixation over III-Nitride Nanowires Assisted by Ruthenium Clusters of Low Atomicity.

机构信息

Department of Chemistry and FQRNT Center for Green Chemistry and Catalysis, McGill University, 801 Sherbrooke Street West, Montreal, QC, H3A 0B8, Canada.

Department of Electrical and Computer Engineering, McGill University, 3480 University Street, Montreal, Québec, H3A 0E9, Canada.

出版信息

Angew Chem Int Ed Engl. 2017 Jul 17;56(30):8701-8705. doi: 10.1002/anie.201703301. Epub 2017 Jun 23.

DOI:10.1002/anie.201703301
PMID:28598586
Abstract

In many heterogeneous catalysts, the interaction of supported metal species with a matrix can alter the electronic and morphological properties of the metal and manipulate its catalytic properties. III-nitride semiconductors have a unique ability to stabilize ultra-small ruthenium (Ru) clusters (ca. 0.8 nm) at a high loading density up to 5 wt %. n-Type III-nitride nanowires decorated with Ru sub-nanoclusters offer controlled surface charge properties and exhibit superior UV- and visible-light photocatalytic activity for ammonia synthesis at ambient temperature. A metal/semiconductor interfacial Schottky junction with a 0.94 eV barrier height can greatly facilitate photogenerated electron transfer from III-nitrides to Ru, rendering Ru an electron sink that promotes N≡N bond cleavage, and thereby achieving low-temperature ammonia synthesis.

摘要

在许多多相催化剂中,负载金属物种与基质的相互作用可以改变金属的电子和形态性质,并操纵其催化性质。III 族氮化物半导体具有独特的能力,可以在高负载密度下(高达 5wt%)稳定超小钌(Ru)簇(约 0.8nm)。用 Ru 亚纳米簇修饰的 n 型 III 族氮化物纳米线具有可控的表面电荷特性,并在环境温度下表现出优异的用于氨合成的紫外光和可见光光催化活性。金属/半导体界面肖特基结的势垒高度为 0.94eV,可以极大地促进光生电子从 III 族氮化物转移到 Ru,使 Ru 成为促进 N≡N 键断裂的电子汇,从而实现低温氨合成。

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