Low-cost CuNi-CeO2/rGO as an efficient catalyst for hydrolysis of ammonia borane and tandem reduction of 4-nitrophenol
Low-cost CuNi-CeO2/rGO as an efficient catalyst for hydrolysis of ammonia borane and tandem reduction of 4-nitrophenol
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低成本CuNi-CeO2/rGO作为氨硼烷水解和4-硝基苯酚串联还原的高效催化剂
DOI：
10.1016/j.jallcom.2017.09.075
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发表时间：
2017-12
影响因子：
6.2
通讯作者：
Yong Cheng
中科院分区：
文献类型：
--
作者：
Zhou Ying Hua;Wang Suqin;Wan Yu;Liang Jingjing;Chen Yu;Luo Shizhong;Yong Cheng
低成本、高性能的金属纳米粒子作为储氢材料的催化剂是储氢材料发展的迫切需要。采用简单的共还原法，在室温下将CeO 2掺杂的CuNi纳米粒子固定在还原氧化石墨烯（rGO）表面，并采用ICP-OES、XRD、TEM、SEM-EDS和XPS等技术对其进行了表征。制备了不同金属含量的CuNi-CeO 2/rGO纳米复合材料，并将其用作氨硼烷（NH3 BH 3，AB）在温和条件下水解脱氢的非均相催化剂。CeO 2含量为13.9mol%时，催化剂Cu0.8Ni0.2-CeO 2/rGO具有优异的催化活性，在298 K时的TOF值为34.4·molH 2·molcatalyst-1·min-1。表观活化能计算为19.1 kJ mol−1，甚至低于大多数用于AB脱氢的贵金属基催化剂。研究了不同催化剂浓度、底物浓度和温度下Cu_（0.8）Ni_（0.2）-CeO_2/rGO催化AB水解反应的详细动力学。此外，从AB水解获得的原位氢可以进一步用于还原4-硝基苯酚，在室温下具有8.1 min-1的高TOF值。Cu0.8Ni0.2-CeO 2/rGO的高催化活性可能与CuNi-CeO 2纳米颗粒的小尺寸、金属-金属协同作用以及金属-载体相互作用有关。
Low-cost metallic nanoparticles as catalysts with good performance are highly desired for the development of hydrogen storage materials. In this work, ceria-doped CuNi nanoparticles were successfully immobilized on the surfaces of reduced graphene oxide (rGO) by a simple co-reduction approach in aqueous solution at room temperature, characterized by ICP-OES, XRD, TEM, SEM-EDS and XPS techniques. The as-synthesized CuNi-CeO2/rGO nanocomposites with various metal contents had been employed as heterogeneous catalysts for the hydrolytic dehydrogenation of ammonia borane (NH3BH3, AB) under mild conditions. The optimal catalyst of Cu0.8Ni0.2-CeO2/rGO with CeO2content of 13.9 mol% exhibited an excellent catalytic activity with the exceedingly high TOF value of 34.4·molH2·molcatalyst−1·min−1at 298 K. The apparent activation energy was calculated to be 19.1 kJ mol−1, even lower than most of noble-metal-based catalysts for AB dehydrogenation. The detailed kinetics of AB hydrolysis catalyzed by Cu0.8Ni0.2-CeO2/rGO had been investigated on different concentrations of catalyst, substrate and temperatures. Moreover, the obtainedin situhydrogen from AB hydrolysis can be further applied to reduce 4-nitrophenol with a high TOF value of 8.1 min−1at room temperature. The high catalytic activity of Cu0.8Ni0.2-CeO2/rGO would be contributed to the small size of CuNi-CeO2NPs, metal-metal synergy, and the metal-support interaction.
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