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Poison Tolerance to the Selective Hydrogenation of Cinnamaldehyde in Water over an Ordered Mesoporous Carbonaceous Composite Supported Pd Catalyst
Chen, Shangjun; Meng, Li; Chen, Bingxu; Chen, Wenyao; Duan, Xuezhi; Huang, Xing; Zhang, Bingsen; Fu, Haibin; Wan, Ying; Wan, Y (reprint author), Shanghai Normal Univ, Shanghai Key Lab Rare Earth Funct Mat, Minist Educ, Key Lab Resource Chem, Shanghai 200234, Peoples R China.; Wan, Y (reprint author), Shanghai Normal Univ, Dept Chem, Shanghai 200234, Peoples R China.
2017-03-01
发表期刊ACS CATALYSIS
ISSN2155-5435
卷号7期号:3页码:2074-2087
摘要A coordination-assisted pyrolysis procedure was adopted to encapsulate palladium (Pd) nanoparticles in a mesoporous carbonaceous matrix. X-ray diffraction and transmission electron microscopy measurements revealed that approximately 2.5 nm nanoparticles were highly dispersed inside the well-ordered porous framework. High-resolution TEM and temperature-programmed hydride decomposition analysis demonstrated the formation of interstitial carbon in the Pd lattice. Diffuse reflectance infrared Fourier transform spectroscopy indicated that carbon species could be deposited on low-coordinated surface sites of the Pd particles. This catalyst exhibited high activity in the selective hydrogenation of cinnamaldehyde (CAL) at 80 degrees C under an H-2 pressure of 1.0 MPa (turnover frequency (TOF) of 2.4 s(-1)) to produce hydrocinnamyl aldehyde with high selectivity (HCAL; approximately 80%) in water and could be reused eight times with no dear activity loss. A trapping agent poisoning experiment using solid SH-SBA-15 revealed unobvious leaching of Pd into the solution. Exposure to thiourea with a S:Pd ratio of 0.1 resulted in slight activity and undetectable selectivity losses over the current catalyst in the selective hydrogenation of CAL at 80 degrees C under an H2 pressure of 1.0 MPa. However, a 50% activity loss was observed for commercial Pd/C. Even after an increase in the thiourea concentration to a S:Pd ratio of 3, the TOF remained at 1.9 s(-1) with a negligible effect on the HCAL selectivity. Nearly complete deactivation of Pd/C occurred upon high exposure to thiourea. DFT calculations showed that the presence of surface or subsurface carbon can enhance the poison tolerance of the encapsulated Pd catalysts. The enhanced hydrogenation activity and strong poison tolerance are consistent with the interpretation that Pd nanoparticles are modified by carbonaceous deposits.; A coordination-assisted pyrolysis procedure was adopted to encapsulate palladium (Pd) nanoparticles in a mesoporous carbonaceous matrix. X-ray diffraction and transmission electron microscopy measurements revealed that approximately 2.5 nm nanoparticles were highly dispersed inside the well-ordered porous framework. High-resolution TEM and temperature-programmed hydride decomposition analysis demonstrated the formation of interstitial carbon in the Pd lattice. Diffuse reflectance infrared Fourier transform spectroscopy indicated that carbon species could be deposited on low-coordinated surface sites of the Pd particles. This catalyst exhibited high activity in the selective hydrogenation of cinnamaldehyde (CAL) at 80 degrees C under an H-2 pressure of 1.0 MPa (turnover frequency (TOF) of 2.4 s(-1)) to produce hydrocinnamyl aldehyde with high selectivity (HCAL; approximately 80%) in water and could be reused eight times with no dear activity loss. A trapping agent poisoning experiment using solid SH-SBA-15 revealed unobvious leaching of Pd into the solution. Exposure to thiourea with a S:Pd ratio of 0.1 resulted in slight activity and undetectable selectivity losses over the current catalyst in the selective hydrogenation of CAL at 80 degrees C under an H2 pressure of 1.0 MPa. However, a 50% activity loss was observed for commercial Pd/C. Even after an increase in the thiourea concentration to a S:Pd ratio of 3, the TOF remained at 1.9 s(-1) with a negligible effect on the HCAL selectivity. Nearly complete deactivation of Pd/C occurred upon high exposure to thiourea. DFT calculations showed that the presence of surface or subsurface carbon can enhance the poison tolerance of the encapsulated Pd catalysts. The enhanced hydrogenation activity and strong poison tolerance are consistent with the interpretation that Pd nanoparticles are modified by carbonaceous deposits.
部门归属[chen, shangjun ; meng, li ; fu, haibin ; wan, ying] shanghai normal univ, shanghai key lab rare earth funct mat, minist educ, key lab resource chem, shanghai 200234, peoples r china ; [chen, shangjun ; meng, li ; fu, haibin ; wan, ying] shanghai normal univ, dept chem, shanghai 200234, peoples r china ; [chen, bingxu ; chen, wenyao ; duan, xuezhi] east china univ sci & technol, state key lab chem engn, 130 meilong rd, shanghai 200237, peoples r china ; [huang, xing] fritz haber inst max planck soc, dept inorgan chem, faradayweg 4-6, d-14195 berlin, germany ; [zhang, bingsen] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china
关键词C-modified Pd Hydrogenation Poison Tolerance Thermal Reduction
学科领域Chemistry, Physical
资助者State Key Basic Research Program of China [2013CB934102]; NSF of China [21322308]; Ministry of Education of China [PCSIR-T_IRT_16R49, 20123127110004]; International Joint Laboratory on Resource Chemistry of China (IJLRC); Shanghai Sci. & Tech. and Edu. Committee [14YF1409200]
收录类别SCI
语种英语
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/78262
专题中国科学院金属研究所
通讯作者Wan, Y (reprint author), Shanghai Normal Univ, Shanghai Key Lab Rare Earth Funct Mat, Minist Educ, Key Lab Resource Chem, Shanghai 200234, Peoples R China.; Wan, Y (reprint author), Shanghai Normal Univ, Dept Chem, Shanghai 200234, Peoples R China.
推荐引用方式
GB/T 7714
Chen, Shangjun,Meng, Li,Chen, Bingxu,et al. Poison Tolerance to the Selective Hydrogenation of Cinnamaldehyde in Water over an Ordered Mesoporous Carbonaceous Composite Supported Pd Catalyst[J]. ACS CATALYSIS,2017,7(3):2074-2087.
APA Chen, Shangjun.,Meng, Li.,Chen, Bingxu.,Chen, Wenyao.,Duan, Xuezhi.,...&Wan, Y .(2017).Poison Tolerance to the Selective Hydrogenation of Cinnamaldehyde in Water over an Ordered Mesoporous Carbonaceous Composite Supported Pd Catalyst.ACS CATALYSIS,7(3),2074-2087.
MLA Chen, Shangjun,et al."Poison Tolerance to the Selective Hydrogenation of Cinnamaldehyde in Water over an Ordered Mesoporous Carbonaceous Composite Supported Pd Catalyst".ACS CATALYSIS 7.3(2017):2074-2087.
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