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Rational Design of Highly Efficient PdIn–In2O3 Interfaces by a Capture-Alloying Strategy for Benzyl Alcohol Partial Oxidation
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-04-04 , DOI: 10.1021/acsami.3c00810
Peng Bai 1 , Zhenxiang Zhao 1 , Yonghui Zhang 1 , Zhengke He 1 , Yonghui Liu 2 , Chunzheng Wang 1 , Shixingwang Ma 1 , Pingping Wu 1 , Lianming Zhao 2 , Svetlana Mintova 3 , Zifeng Yan 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-04-04 , DOI: 10.1021/acsami.3c00810
Peng Bai 1 , Zhenxiang Zhao 1 , Yonghui Zhang 1 , Zhengke He 1 , Yonghui Liu 2 , Chunzheng Wang 1 , Shixingwang Ma 1 , Pingping Wu 1 , Lianming Zhao 2 , Svetlana Mintova 3 , Zifeng Yan 1
Affiliation
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Well-dispersed PdIn bimetallic alloy nanoparticles (1–4 nm) were immobilized on mesostructured silica by an in situ capture-alloying strategy, and PdIn–In2O3 interfaces were rationally constructed by changing the In2O3 loading and reduction temperature. The catalytic performance for benzyl alcohol partial oxidation was evaluated, and a catalytic synergy was observed. The Pd-rich PdIn–In2O3 interface is prone to be formed on the catalyst with a low In2O3 loading after being reduced at 300 °C. It was demonstrated that the Pd-rich PdIn–In2O3 interface was more active for benzyl alcohol partial oxidation than In-rich Pd2In3 species, which was likely to be formed at a high reduction temperature (400 °C). The high catalytic activity on the Pd-rich PdIn–In2O3 interface was attributed to the exposure of more Pd-enriched active sites, and an optimized PdIn–In2O3/Pd assemble ratio enhanced the oxygen transfer during partial oxidation. The density functional theory (DFT) calculation confirmed that the Pd-rich Pd3In1(111)–In2O3 interface facilitated the activation of oxygen molecules, resulting in high catalytic activity.
中文翻译：
通过苯甲醇部分氧化的捕获合金化策略合理设计高效 PdIn-In2O3 界面
通过原位捕获合金策略将分散良好的 PdIn 双金属合金纳米粒子 (1–4 nm) 固定在介观结构二氧化硅上，并通过改变 In 2 O 3负载和还原温度合理构建PdIn–In 2 O 3界面。评估了苯甲醇部分氧化的催化性能，并观察到催化协同作用。在300℃还原后， In 2 O 3负载量低的催化剂上容易形成富含Pd的PdIn- In 2 O 3界面。结果表明，富钯 PdIn–In 2 O 3界面对苯甲醇部分氧化比富含 In 的 Pd 2 In 3物种更活跃，这可能是在高还原温度 (400 °C) 下形成的。富 Pd 的 PdIn-In 2 O 3界面上的高催化活性归因于更多富 Pd 活性位点的暴露，优化的 PdIn-In 2 O 3 /Pd 组装比增强了部分氧化过程中的氧转移。密度泛函理论（DFT）计算证实富含Pd的Pd 3 In 1 (111)–In 2 O 3界面促进了氧分子的活化，从而产生高催化活性。
更新日期：2023-04-04
中文翻译：
通过苯甲醇部分氧化的捕获合金化策略合理设计高效 PdIn-In2O3 界面
通过原位捕获合金策略将分散良好的 PdIn 双金属合金纳米粒子 (1–4 nm) 固定在介观结构二氧化硅上，并通过改变 In 2 O 3负载和还原温度合理构建PdIn–In 2 O 3界面。评估了苯甲醇部分氧化的催化性能，并观察到催化协同作用。在300℃还原后， In 2 O 3负载量低的催化剂上容易形成富含Pd的PdIn- In 2 O 3界面。结果表明，富钯 PdIn–In 2 O 3界面对苯甲醇部分氧化比富含 In 的 Pd 2 In 3物种更活跃，这可能是在高还原温度 (400 °C) 下形成的。富 Pd 的 PdIn-In 2 O 3界面上的高催化活性归因于更多富 Pd 活性位点的暴露，优化的 PdIn-In 2 O 3 /Pd 组装比增强了部分氧化过程中的氧转移。密度泛函理论（DFT）计算证实富含Pd的Pd 3 In 1 (111)–In 2 O 3界面促进了氧分子的活化，从而产生高催化活性。
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