Skeletal Ni catalysts prepared from Ni–Al alloys rapidly quenched at different rates: Texture, structure and catalytic performance in chemoselective hydrogenation of 2-ethylanthraquinone

Skeletal Ni catalysts prepared from Ni–Al alloys rapidly quenched at different rates: Texture, structure and catalytic performance in chemoselective hydrogenation of 2-ethylanthraquinone
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DOI:
10.1016/j.jcat.2005.11.001
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发表时间:
2006
影响因子:
7.3
通讯作者:
Huarong Hu;Fuzhong Xie;Yan Pei;M. Qiao;Shirun Yan;Heyong He;Kangnian Fan;Hexing Li;B. Zong;Xiaoxin Zhang
Huarong Hu;Fuzhong Xie;Yan Pei;M. Qiao;Shirun Yan;Heyong He;Kangnian Fan;Hexing Li;B. Zong;Xiaoxin Zhang
中科院分区:
化学1区
文献类型:
--
作者:
Huarong Hu;Fuzhong Xie;Yan Pei;M. Qiao;Shirun Yan;Heyong He;Kangnian Fan;Hexing Li;B. Zong;Xiaoxin Zhang

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对快速淬火镍铝合金碱浸法制备骨架镍催化剂(RQ Ni)进行了系统表征,重点研究了制备过程中冷却速率的影响。结果表明,RQ Ni催化剂的残铝含量、织构、结构、表面氢的种类和活性位点均可通过Ni - Al合金的冷却速率来控制。在2-乙基蒽醌(eAQ)液相加氢过程中,冷却速率较高的RQ Ni催化剂有利于羰基的加氢,延缓了芳环的饱和和降解产物的形成,从而提高了H2O2的产率。基于表征,选择性的提高是由于强化学吸附的氢占主导地位,对芳香环的氢化无活性,以及残余金属Al和Ni之间的电子相互作用,有利于催化剂上eAQ的羰基键构型。
Skeletal Ni catalysts (RQ Ni) prepared by alkali leaching of rapidly quenched Ni–Al alloys have been systematically characterized, focusing on the effect of the cooling rate during alloy preparation. It is found that the residual Al content, texture, structure, surface hydrogen species, and active sites of the RQ Ni catalysts can be controlled by the cooling rate of the Ni–Al alloys. In liquid-phase hydrogenation of 2-ethylanthraquinone (eAQ), the RQ Ni catalyst with higher cooling rate favors hydrogenation of the carbonyl group and retards the saturation of the aromatic ring and the formation of the degradation products, thus leading to a higher yield of H2O2. Based on the characterizations, the improved selectivity is ascribed to the dominant population of strongly chemisorbed hydrogen, which is inactive for the hydrogenation of the aromatic ring, along with the electronic interaction between residual metallic Al and Ni, favoring a carbonyl group-bonded configuration of eAQ on the catalyst.