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用于在温和条件下将硝基苯高效催化氢化为苯胺的三维网络状Pd-Ni/γ-Al₂O₃催化剂

Three-Dimensional Network Pd-Ni/γ-AlO Catalysts for Highly Active Catalytic Hydrogenation of Nitrobenzene to Aniline under Mild Conditions.

作者信息

Jiang Yang, Li Qian, Li Xi, Wang Xinyi, Dong Sen, Li Jianhua, Hou Li, Jiao Tifeng, Wang Yatao, Gao Faming

机构信息

Hebei Key Laboratory of Applied Chemistry, School of Environmental and Chemical Engineering, Yanshan University, 438West Hebei Street, Qinhuangdao 066004, China.

Coal Chemical R&D Center of Kailuan Group, Tangshan 063611, China.

出版信息

ACS Omega. 2021 Apr 1;6(14):9780-9790. doi: 10.1021/acsomega.1c00441. eCollection 2021 Apr 13.

DOI:10.1021/acsomega.1c00441
PMID:33869958
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8047756/
Abstract

In view of the current situation of high cost and low catalytic efficiency of the commercial Pd-based catalysts, adding transition metals (Ni, Co, etc.) to form the Pd-M bimetallic catalyst not only reduces the consumption of Pd but also greatly improves the catalytic activity and stability, which has attracted increasing attention. In this work, the three-dimensional network Pd-Ni bimetallic catalysts were prepared successfully by a liquid-phase in situ reduction method with the hydroxylated γ-AlO as the support. Through investigating the effects of the precursor salt amount, reducing agent concentration, stabilizer concentration, and reducing stirring time on the synthesis of the Pd-Ni nanocatalyst, the three-dimensional network Pd-Ni bimetallic nanostructures with four different atomic ratios were prepared under an optimal condition. The obtained wire-like Pd-Ni catalysts have a uniform diameter size of about 5 nm and length up to several microns. After closely combining with the hydroxylated γ-AlO, the supported Pd-Ni/γ-AlO catalysts exhibit nearly 100% conversion rate and selectivity for the hydrogenation of nitrobenzene to aniline at low temperature and normal pressure. The stability testing of the supported Pd-Ni/γ-AlO catalysts shows that the conversion rate still remained above 99% after 10 cycles. There is no doubt that the supported catalysts show significant catalytic efficiency and recyclability, which provides important theoretical basis and technical support for the preparation of low-cost, highly efficient catalysts for the hydrogenation of nitrobenzene to aniline.

摘要

鉴于目前商业钯基催化剂成本高、催化效率低的现状,添加过渡金属(镍、钴等)形成钯 - 金属双金属催化剂不仅降低了钯的消耗,还大大提高了催化活性和稳定性,这引起了越来越多的关注。在本工作中,以羟基化γ - 氧化铝为载体,通过液相原位还原法成功制备了三维网络状钯 - 镍双金属催化剂。通过研究前驱体盐量、还原剂浓度、稳定剂浓度和还原搅拌时间对钯 - 镍纳米催化剂合成的影响,在最佳条件下制备了四种不同原子比的三维网络状钯 - 镍双金属纳米结构。所制备的线状钯 - 镍催化剂直径均匀,约为5 nm,长度可达数微米。与羟基化γ - 氧化铝紧密结合后,负载型钯 - 镍/γ - 氧化铝催化剂在低温常压下对硝基苯加氢制苯胺表现出近100%的转化率和选择性。负载型钯 - 镍/γ - 氧化铝催化剂的稳定性测试表明,经过10次循环后转化率仍保持在99%以上。毫无疑问,负载型催化剂显示出显著的催化效率和可回收性,这为制备用于硝基苯加氢制苯胺的低成本、高效催化剂提供了重要的理论依据和技术支持。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/20bf68203c21/ao1c00441_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/e13907803377/ao1c00441_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/74283919adc6/ao1c00441_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/1ebf66785083/ao1c00441_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/661ab6e359a1/ao1c00441_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/992a478814b0/ao1c00441_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/20bf68203c21/ao1c00441_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/e13907803377/ao1c00441_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/74283919adc6/ao1c00441_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/1ebf66785083/ao1c00441_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/661ab6e359a1/ao1c00441_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/992a478814b0/ao1c00441_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/db4f/8047756/20bf68203c21/ao1c00441_0006.jpg

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