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在TiO表面接枝超交联聚合物以锚定超细钯纳米颗粒:显著提高将CO光催化还原为CH的效率和选择性。

Grafting Hypercrosslinked Polymers on TiO Surface for Anchoring Ultrafine Pd Nanoparticles: Dramatically Enhanced Efficiency and Selectivity toward Photocatalytic Reduction of CO to CH.

作者信息

Zhan Zhen, Wang Heng, Huang Qi, Li Shuqing, Yi Xiaoxuan, Tang Qian, Wang Jingyu, Tan Bien

机构信息

Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Luoyu Road No. 1037, Wuhan, 430074, China.

出版信息

Small. 2022 Jan;18(1):e2105083. doi: 10.1002/smll.202105083. Epub 2021 Nov 26.

DOI:10.1002/smll.202105083
PMID:34825480
Abstract

Metal deposition with photocatalyst is a promising way to surmount the restriction of fast e /h recombination to improve the photocatalytic performance. However, the improvement remains limited by the existing strategies adopted for depositing metal particles due to the serious aggregation and large unconnected area on photocatalyst surface. Here, a strategy is proposed by directly grafting hypercrosslinked polymers (HCPs) on TiO surface to construct Pd-HCPs-TiO composite with uniform dispersion of ultrafine Pd nanoparticles on HCPs surface. This composite with surface area of 373 m g exhibits improved photocatalytic CO conversion efficiency to CH with an evolution rate of 237.4 µmol g h and selectivity of more than 99.9%. The enhancement can be ascribed to the grafted porous HCPs with high surface area and N heteroatom on TiO surface for the stabilization of Pd nanoparticles, favoring the electron transfer and CO adsorption for selective CH production. This strategy may hold the promise for design and construction of porous organic polymer with semiconductor for efficient photocatalytic conversion.

摘要

光催化剂金属沉积是克服快速电子/空穴复合限制以提高光催化性能的一种有前途的方法。然而,由于光催化剂表面金属颗粒严重聚集和大面积未连接区域,采用现有策略沉积金属颗粒时,性能提升仍然有限。在此,提出一种策略,通过在TiO表面直接接枝超交联聚合物(HCPs)来构建Pd-HCPs-TiO复合材料,使超细Pd纳米颗粒均匀分散在HCPs表面。这种表面积为373 m²/g的复合材料表现出改善的光催化CO转化为CH₄的效率,析出速率为237.4 µmol g⁻¹ h⁻¹,选择性超过99.9%。这种增强可归因于TiO表面接枝的具有高表面积和N杂原子的多孔HCPs,用于稳定Pd纳米颗粒,有利于电子转移和CO吸附以选择性生成CH₄。该策略有望用于设计和构建具有半导体的多孔有机聚合物以实现高效光催化转化。

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