CeO2 结构工程助推 Au/CeO2 纳米催化剂用于硝基苯绿色选择性加氢,Nanoscale Horizons

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CeO2 结构工程助推 Au/CeO2 纳米催化剂用于硝基苯绿色选择性加氢
Nanoscale Horizons ( IF 8.0 ) Pub Date : 2023-03-23 , DOI: 10.1039/d3nh00103b
Junqing Ye _{1,

2} , Meizan Jing ₃ , Yu Liang ₁ , Wenjin Li ₁ , Wanting Zhao ₁ , Jianying Huang _{4,

5} , Yuekun Lai _{4,

5} , Weiyu Song ₃ , Jian Liu ₃ , Jian Sun _{1,

6}

Affiliation

探索纳米级结构工程的生态友好且具有成本效益的策略对于促进多相催化非常重要，但仍面临长期挑战。在此，多功能多酚单宁酸，一种含有儿茶酚和没食子酰物种的低成本天然生物质，被用作绿色还原剂、螯合剂和稳定剂来制备分散在不同形状的 CeO 2_载体（例如，杆、花、立方体和八面体）。系统表征表明 Au/CeO ₂棒具有最高的氧空位密度和 Ce( III）比例，有利于金属活性位点的分散和稳定。使用异丙醇作为氢转移试剂，深入了解了具有不同CeO _{2形貌的Au/CeO}₂催化剂在催化硝基苯转移加氢反应中的构效关系。值得注意的是，催化性能遵循以下顺序：Au/CeO ₂ -rod (110), (100), (111) > Au/CeO ₂ -flower (100), (111) > Au/CeO ₂ -cube (100) > Au/CeO ₂ -octa (111)。金/二氧化_铈-rod 在最佳条件下显示出最高的 100% 硝基苯转化率和出色的稳定性。此外，DFT计算表明硝基苯分子在Au/CeO ₂ (110)表面具有合适的吸附能和更好的异丙醇脱氢能力。基于该结果提出了催化硝基苯转移加氢的反应途径和协同催化机理。这项工作表明，CeO ₂结构工程是制造用于硝基苯加氢的先进环保材料的有效策略。

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Structure engineering of CeO2 for boosting the Au/CeO2 nanocatalyst in the green and selective hydrogenation of nitrobenzene

Exploring eco-friendly and cost-effective strategies for structure engineering at the nanoscale is important for boosting heterogeneous catalysis but still under a long-standing challenge. Herein, multifunctional polyphenol tannic acid, a low-cost natural biomass containing catechol and galloyl species, was employed as a green reducing agent, chelating agent, and stabilizer to prepare Au nanoparticles, which were dispersed on different-shaped CeO₂ supports (e.g., rod, flower, cube, and octahedral). Systematic characterizations revealed that Au/CeO₂-rod had the highest oxygen vacancy density and Ce(III) proportion, favoring the dispersion and stabilization of the metal active sites. Using isopropanol as a hydrogen-transfer reagent, deep insights into the structure–activity relationship of the Au/CeO₂ catalysts with various morphologies of CeO₂ in the catalytic nitrobenzene transfer hydrogenation reaction were gained. Notably, the catalytic performance followed the order: Au/CeO₂-rod (110), (100), (111) > Au/CeO₂-flower (100), (111) > Au/CeO₂-cube (100) > Au/CeO₂-octa (111). Au/CeO₂-rod displayed the highest conversion of 100% nitrobenzene and excellent stability under optimal conditions. Moreover, DFT calculations indicated that nitrobenzene molecules had a suitable adsorption energy and better isopropanol dehydrogenation capacity on the Au/CeO₂ (110) surface. A reaction pathway and the synergistic catalytic mechanism for catalytic nitrobenzene transfer hydrogenation are proposed based on the results. This work demonstrates that CeO₂ structure engineering is an efficient strategy for fabricating advanced and environmentally benign materials for nitrobenzene hydrogenation.

更新日期：2023-03-23

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