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一种新型碳载体:少层石墨炔修饰的碳纳米管捕获金属簇作为有效的金属负载催化剂。

A Novel Carbon Support: Few-Layered Graphdiyne-Decorated Carbon Nanotubes Capture Metal Clusters as Effective Metal-Supported Catalysts.

作者信息

Lv Yan, Wu Xueyan, Lin He, Li Jiaxin, Zhang Hongbo, Guo Jixi, Jia Dianzeng, Zhang Hongmei

机构信息

Key Laboratory of Energy Materials Chemistry, Ministry of Education; Key Laboratory of Advanced Functional Materials, Autonomous Region, Institute of Applied Chemistry, College of Chemistry, Xinjiang University, Urumqi, Xinjiang, 830046, P.R. China.

出版信息

Small. 2021 Mar;17(12):e2006442. doi: 10.1002/smll.202006442. Epub 2021 Mar 3.

Abstract

Carbon-supported metal nanocatalysts have received substantial attention for heterogeneous catalysis in industry. Hunting for suitable and impactful carbon supports that have strong interactions with metal nanocatalyst is a matter of great urgency. Herein, a well-designed graphdiyne layer decorated on the carbon nanotubes sidewalls (CNT@GDY) serves as a novel carbon support. This unique hybrid structure effectively traps platinum and palladium atomic clusters (Pt/Pd-ACs) with dimensions of 0.65 nm and 1.05 nm uniformly and firmly, forming novel carbon-supported metal nanocatalysts (Pt(Pd)-ACs/CNT @ GDY) for efficient hydrogen generation and aromatic nitroreduction, respectively. The Pt-ACs/CNT@GDY can deliver an HER current density of 10 mA cm with a small overpotential of 23 mV in 0.5 M H SO , showing a greatly enhanced mass activity, intrinsic activity than the commercial Pt/C catalyst. The Pd-ACs/CNT@GDY also exhibits excellent catalytic activity and a high turnover frequency of 38.0 min for aromatic nitroreduction. The carbon support turns out to possess excellent conductivity, abundant and uniform reactive sites, low redox potential, more negative surface and large specific surface area as well as a strong interaction with ACs, as anticipated in ideal supports, which can be applied in other metal-supported catalysts.

摘要

碳负载金属纳米催化剂在工业多相催化中受到了广泛关注。寻找与金属纳米催化剂具有强相互作用的合适且有影响力的碳载体是当务之急。在此,一种精心设计的修饰在碳纳米管侧壁上的石墨炔层(CNT@GDY)作为一种新型碳载体。这种独特的杂化结构有效地均匀且牢固地捕获尺寸为0.65纳米和1.05纳米的铂和钯原子簇(Pt/Pd-ACs),分别形成用于高效产氢和芳香族硝基还原的新型碳负载金属纳米催化剂(Pt(Pd)-ACs/CNT@GDY)。在0.5 M H₂SO₄中,Pt-ACs/CNT@GDY能在23 mV的小过电位下提供10 mA cm⁻²的析氢电流密度,与商业Pt/C催化剂相比,显示出大大增强的质量活性和本征活性。Pd-ACs/CNT@GDY在芳香族硝基还原中也表现出优异的催化活性和38.0 min⁻¹的高周转频率。正如理想载体所预期的那样,该碳载体具有优异的导电性、丰富且均匀的反应位点、低氧化还原电位、更负的表面和大比表面积以及与ACs的强相互作用,可应用于其他金属负载催化剂。

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