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碳量子点@钯-锡硫纳米复合物:CQDs@Pd 纳米簇在增强芳香族硝基化合物光催化还原中的作用。

Carbon quantum dots @ Pd-SnS nanocomposite: The role of CQDs @ Pd nanoclusters in enhancing photocatalytic reduction of aromatic nitro compounds.

机构信息

Hubei Collaborative Innovation Center for Advanced Organochemical Materials, Ministry-of-Education Key Laboratory for the Synthesis and Applications of Organic Functional Molecules, Hubei University, Wuhan 430062, PR China.

Hubei Collaborative Innovation Center for Advanced Organochemical Materials, Ministry-of-Education Key Laboratory for the Synthesis and Applications of Organic Functional Molecules, Hubei University, Wuhan 430062, PR China.

出版信息

J Colloid Interface Sci. 2019 Nov 1;555:423-430. doi: 10.1016/j.jcis.2019.08.002. Epub 2019 Aug 2.

Abstract

2D layered SnS is one of the most popular semiconductor photocatalysts. However, its performance on photocatalytic reduction of aromatic nitro compounds is unsatisfactory, due to charge carrier recombination and weak adsorption of active hydrogen from the hydrolysis of NaBH. Herein, we have prepared CQDs @ Pd nanoclusters with Pd nanoparticles below 5 nm through an in-situ reducing Pd(Ⅱ) with CQDs containing some oxygen-containing groups at first. CQDs @ Pd-SnS is achieved through a strong interaction of sulfur ions bonding on nanometric Pd surface. The composite shows a stable and efficient visible-light-driven catalytic reduction of aromatic nitro compounds in HO and NaBH. Under 40 min visible light irradiation, the conversion rate of 4-NP attains 99.7% on CQDs @ Pd-SnS. The first order reaction rate constant is 0.0332 min, 586.5, 202.4 and 31.9 times that on SnS, CQDs-SnS and Pd-SnS in the condition of 20 mg·L 4-NP and excess NaBH, respectively. The significant enhancement is ascribed to CQDs @ Pd promoting the charge carrier separation on SnS and increasing the adsorption of active hydrogen from the hydrolysis of NaBH.

摘要

二维层状 SnS 是最受欢迎的半导体光催化剂之一。然而,由于载流子复合和来自 NaBH 水解的活性氢的弱吸附,其在芳香族硝基化合物的光催化还原性能并不令人满意。在此,我们通过首先用含有一些含氧基团的 CQDs 将 Pd(Ⅱ)原位还原,制备了粒径小于 5nm 的 CQDs@Pd 纳米团簇。通过硫离子与纳米 Pd 表面键合的强相互作用,得到了 CQDs@Pd-SnS。该复合材料在可见光照射下,在 HO 和 NaBH 中表现出稳定高效的芳香族硝基化合物光催化还原活性。在 40min 可见光照射下,CQDs@Pd-SnS 上 4-NP 的转化率达到 99.7%。在 20mg·L 的 4-NP 和过量 NaBH 的条件下,CQDs@Pd-SnS 的一级反应速率常数分别是 SnS、CQDs-SnS 和 Pd-SnS 的 0.0332 min、586.5、202.4 和 31.9 倍。显著的增强归因于 CQDs@Pd 促进了 SnS 上载流子的分离,并增加了来自 NaBH 水解的活性氢的吸附。

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