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Highly active bifunctional Pd-Co9S8/S-CNT catalysts for selective hydrogenolysis of 5-hydroxymethylfurfural to 2,5-dimethylfuran
Molecular Catalysis ( IF 4.6 ) Pub Date : 2019-12-30 , DOI: 10.1016/j.mcat.2019.110756
Weiping Liao , Zhiguo Zhu , Naimeng Chen , Ting Su , Changliang Deng , Yuchao Zhao , Wanzhong Ren , Hongying Lü

A series of Pd-Co bimetallic catalysts were smoothly synthesized using sulfur-modified carbon nanotubes (S-CNT) as support by impregnation method. Those catalysts were characterized by XRD, XPS, TEM, SEM, H2-TPR, TGA, and nitrogen adsorption-desorption. Selective catalytic hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF) was realized over these synthesized sulfur-modified Pd-Co bimetallic supported on carbon nanotubes (PdCox/S-CNT) under mild conditions. Among them, PdCo8/S-CNT catalyst possessed extremely active and selective for the production of DMF, giving 96.0 % conversion of HMF with 83.7 % selectivity to DMF at the temperature of 120 °C with 0.3 MPa H2 for 13 h. It is found that the formed Co9S8 species are related to the high catalytic activity in PdCo8/S-CNT. Control experiments for evaluating the roles of palladium and Co9S8 revealed that Pd catalyzed the hydrogenation of the aldehyde group in HMF whereas Co9S8 was beneficial for hydrogenolysis of the hydroxy group in HMF. The remarkable hydrogenolysis/hydrogenation performance of the bifunctional Pd-Co9S8/S-CNT was due to support-enhanced adsorption effect and the effective synergy between highly dispersed metallic Pd and the Co9S8 nanoparticles.



中文翻译:

高活性双官能Pd-Co 9 S 8 / S-CNT催化剂,用于5-羟甲基糠醛选择性氢解为2,5-二甲基呋喃

以硫改性碳纳米管(S-CNT)为载体,通过浸渍法顺利合成了一系列Pd-Co双金属催化剂。这些催化剂通过XRD,XPS,TEM,SEM,H 2 -TPR,TGA和氮吸附-脱附来表征。在温和的条件下,在碳纳米管(PdCo x / S-CNT)上负载的这些合成的硫改性的Pd-Co双金属化合物上实现了5-羟甲基糠醛 HMF)选择性催化氢解为2,5-二甲基呋喃(DMF)。其中,PdCo 8 / S-CNT催化剂对DMF的生产具有极高的活性和选择性,在120℃,0.3 MPa H 2的温度下,HMF的转化率为96.0%,对DMF的选择性为83.7%。持续13小时。发现形成的Co 9 S 8物种与PdCo 8 / S-CNT中的高催化活性有关。评估钯和Co 9 S 8的作用的对照实验表明,钯催化HMF中醛基的氢化,而Co 9 S 8有助于HMF中羟基的氢解。双功能Pd-Co 9 S 8 / S-CNT的显着氢解/氢化性能归因于载体增强的吸附作用以及高度分散的金属Pd与Co 9 S 8纳米粒子之间的有效协同作用。

更新日期:2019-12-31
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