AuFe3@Pd/γ-Fe2O3 纳米片作为原位可再生高效加氢催化剂,ACS Nano

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AuFe3@Pd/γ-Fe2O3 纳米片作为原位可再生高效加氢催化剂
ACS Nano ( IF 15.8 ) Pub Date : 2023-04-19 , DOI: 10.1021/acsnano.3c00745
Zongshan Zhao _{1,

2} , Yanhen Wu _{1,

2} , Wei Ran _{1,

3} , Huachao Zhao ₁ , Xiaotian Yu ₁ , Jie-Fang Sun ₄ , Guangzhi He ₁ , Jingfu Liu _{1,

2,

3} , Rui Liu _{1,

2,

3} , Guibin Jiang _{1,

2,

3}

Affiliation

多相Pd催化剂在化学工业中起着举足轻重的作用；然而，它长期受到S ^{2-或其他强吸附物诱导表面中毒的困扰。}_{在此，我们报告了 AuFe 3} @Pd/γ-Fe ₂ O ₃纳米片 (NSs) 作为原位可再生和高活性加氢催化剂的开发。中毒后，Pd 单层位点可以在环境条件下完全氧化再生，这是由来自表面缺陷的•OH 自由基/富含 Fe _Tetra空位的 γ-Fe ₂ O _3引发的NSs 通过类芬顿途径。实验和理论分析均表明，对于电子和几何效应，2-3 nm AuFe ₃金属间纳米团簇核促进了反应物在Pd位点上的吸附；此外，它还降低了 Pd 对 •OH 自由基的亲和力，从而增强了它们在氧化再生过程中的稳定性。当填充到石英砂固定床催化剂柱中时，AuFe ₃ @Pd/γ-Fe ₂ O ₃NSs 在碳-卤键氢化方面具有很高的活性，这是去除饮用水中微污染物和从重度污染废水中回收资源的关键步骤，并且可以承受十轮再生。通过最大限度地利用超薄金属氧化物 NSs 和金属间纳米团簇和单层 Pd，目前的研究展示了开发用于液体催化的可持续 Pd 催化剂的综合策略。

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AuFe3@Pd/γ-Fe2O3 Nanosheets as an In Situ Regenerable and Highly Efficient Hydrogenation Catalyst

Heterogenous Pd catalysts play a pivotal role in the chemical industry; however, it is plagued by S^2– or other strong adsorbates inducing surface poisoning long term. Herein, we report the development of AuFe₃@Pd/γ-Fe₂O₃ nanosheets (NSs) as an in situ regenerable and highly active hydrogenation catalyst. Upon poisoning, the Pd monolayer sites could be fully and oxidatively regenerated under ambient conditions, which is initiated by •OH radicals from surface defect/Fe_Tetra vacancy-rich γ-Fe₂O₃ NSs via the Fenton-like pathway. Both experimental and theoretical analyses demonstrate that for the electronic and geometric effect, the 2–3 nm AuFe₃ intermetallic nanocluster core promotes the adsorption of reactant onto Pd sites; in addition, it lowers Pd’s affinity for •OH radicals to enhance their stability during oxidative regeneration. When packed into a quartz sand fixed-bed catalyst column, the AuFe₃@Pd/γ-Fe₂O₃ NSs are highly active in hydrogenating the carbon–halogen bond, which comprises a crucial step for the removal of micropollutants in drinking water and recovery of resources from heavily polluted wastewater, and withstand ten rounds of regeneration. By maximizing the use of ultrathin metal oxide NSs and intermetallic nanocluster and monolayer Pd, the current study demonstrates a comprehensive strategy for developing sustainable Pd catalysts for liquid catalysis.

更新日期：2023-04-19

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