Selective hydrogenation using palladium bioinorganic catalyst
Selective hydrogenation using palladium bioinorganic catalyst
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DOI：
10.1016/j.apcatb.2016.05.060
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发表时间：
2016-12
影响因子：
22.1
通讯作者：
Junyan Zhu;J. Wood;K. Deplanche;I. Mikheenko;L. Macaskie
中科院分区：
文献类型：
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作者：
Junyan Zhu;J. Wood;K. Deplanche;I. Mikheenko;L. Macaskie
钯生物无机催化剂（bio-Pd）使用细菌（脱硫脱硫弧菌和大肠杆菌）将Pd（II）弧菌还原为生物支架Pd（0）纳米颗粒（NPs）来制造。使用电子显微镜和X射线粉末衍射方法检查形成的Pd NP：5重量% Pd的负载显示出约4 nm的平均粒度。在两个加氢反应中与常规负载的Pd催化剂（Pd/Al 2 O3）的催化活性进行比较，所制备的生物Pd NPs对两种细菌的催化活性。使用Langmuir-Hinshelwood表达式拟合不同氢化产物的浓度曲线。在2-戊炔氢化反应中，5 wt%的PdE. coli在20 min内实现了100%的2-戊炔转化率，并产生了10.1 ± 0.7 × 10− 2 mol L− 1的所需顺式-2-戊烯;相比之下，5 wt%的Pd/Al 2 O3在40 min后产生了6.5 ± 0.4 × 10− 2 mol L− 1的顺式-2-戊烯。在大豆油的无溶剂氢化中，使用5 wt%的PdE. coli在5 h后产生1.03 ± 0.04 mol L− 1的顺式-C18：1和0.26 ± 0.03 mol L−1的反式-C18：1（后者比5 wt%的Pd/Al 2 O3少约50%）。使用bio-PdE. coliandbio-PdD. sulfosicans获得了类似的结果。Bio-Pd的结论是具有较低的顺式-反式异构化的优势，在氢化的炔/烯烃。因此，生物制造是一种具有环境吸引力的、可规模化的和容易替代传统非均相催化剂用于工业氢化过程的方法。脱硫菌不便于规模化生长，但浪费E.大肠杆菌由各种工业过程产生。“第二生命”（即从中试规模的生物氢生产过程中回收）E.大肠杆菌细胞用于制备生物Pd催化剂。虽然'生物钯secondlife'给出了一个较慢的2-戊炔和大豆油的转化率相比，生物钯从目的生长的细胞，它表现出较高的选择性，顺式异构体产品。
Palladium bioinorganic catalyst (bio-Pd) was manufactured using bacteria (Desulfovibrio desulfuricans and Escherichia coli)viathe reduction of Pd(II) to bio-scaffolded Pd(0) nanoparticles (NPs). The formed Pd NPs were examined using electron microscopy and X-ray powder diffraction methods: a loading of 5 wt% Pd showed an average particle size of ∼4 nm. The catalytic activities of the prepared bio-Pd NPs on both bacteria were compared in two hydrogenation reactions with that of a conventionally supported Pd catalyst (Pd/Al2O3). Concentration profiles of the different hydrogenation products were fitted using a Langmuir-Hinshelwood expression. In 2-pentyne hydrogenation, 5 wt% PdE.coliachieved 100% of 2-pentyne conversion in 20 mins and produced 10.1 ± 0.7 × 10−2mol L−1of desiredcis-2-pentene; in contrast 5 wt% Pd/Al2O3yielded 6.5 ± 0.4 × 10−2mol L−1ofcis-2-pentene after 40 mins. In the solvent-free hydrogenation of soybean oil, the use of 5 wt% PdE.coliyieldedcis-C18:1 of 1.03 ± 0.04 mol L−1andtrans-C18:1 of 0.26 ± 0.03 mol L−1(∼50% less of the latter than 5 wt% Pd/Al2O3) after 5 h. Similar results were obtained using bio-PdE.coliand bio-PdD.desulfuricans. Bio-Pd was concluded to have the advantage of a lowercis-transisomerisation in hydrogenation of alkyne/alkenes. Hence biomanufacturing is an environmentally attractive, scalable and facile alternative to conventional heterogeneous catalyst for application in industrial hydrogenation processes.D. desulfuricansis inconvenient to grow at scale but wastes ofE. coliare produced from various industrial processes. ‘Second life’ (i.e. recycled from a pilot scale biohydrogen production process)E. colicells were used to make bio-Pd catalysts. Although ‘bio-Pdsecondlife’gave a slower conversion rate of 2-pentyne and soybean oil compared to bio-Pd from purpose-grown cells it showed a higher selectivity to thecis-isomer product.