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Design of Efficient Noble Metal Free Copper‐Promoted Nickel‐Ceria‐Zirconia Nanocatalyst for Bio‐Fuel Upgrading
ChemistrySelect ( IF 1.9 ) Pub Date : 2018-06-13 , DOI: 10.1002/slct.201800896 Ramana Singuru 1, 2 , Jihyeon Lee 3 , Karnekanti Dhanalaxmi 1, 2 , Benjaram M. Reddy 1, 2 , Kwangjin An 3 , John Mondal 1, 2
ChemistrySelect ( IF 1.9 ) Pub Date : 2018-06-13 , DOI: 10.1002/slct.201800896 Ramana Singuru 1, 2 , Jihyeon Lee 3 , Karnekanti Dhanalaxmi 1, 2 , Benjaram M. Reddy 1, 2 , Kwangjin An 3 , John Mondal 1, 2
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A new series of noble metal free bimetallic Cu−Ni supported ceria‐zirconia catalysts (Cu−Ni/CZ) has been developed with various Cu/Ni ratios by a simple co‐precipitation/impregnation method. Aqueous‐phase hydrodeoxygenation (HDO) of vanillin a typical compound of lignin‐derived bio‐oil, in promoting biomass refining was carried out to investigate catalytic performances under 25 bar of H2 pressure at 160oC. All the as‐synthesized catalysts were thoroughly characterised employing powder XRD, Raman spectroscopy, H2‐TPR, HR‐TEM, HAADF‐STEM, EDS Mapping, and XPS. It was found that 15 wt% Cu on Ni/CZ (Cu−Ni/CZ−B) nanocomposite enhanced activity significantly in comparison with other bimetallic or monometallic catalysts, exhibiting ∼98% of vanillin conversion and ∼94% of selectivity toward 2‐methoxy‐4‐methylphenol as a desired product. The Cu−Ni/CZ−B catalyst shows ∼4‐fold increase in activity compared with Cu−Ni/CeO2 and Cu−Ni/ZrO2, the mono oxide supported counterparts. The superior catalytic performance with improved stability were explained by synergistic effects at the interfaces of each species, in which electron interactions between Ni, Cu, and ceria‐zirconia support generated novel active sites. XRD and HR‐TEM revealed that Cu−Ni bimetallic phases were created on the ceria‐zirconia, which were responsible for enhancement of catalytic performance with no significant drop in catalytic activity with desired product selectivity for eleven successive catalytic cycles demonstrating the excellent stability and reproducibility of this catalyst system.
中文翻译：
高效无贵金属铜促进镍-铈-锆-锆纳米催化剂的生物燃料升级设计
通过简单的共沉淀/浸渍方法，已经开发出了一系列新的不含贵金属的双金属负载Cu-Ni的二氧化铈-氧化锆催化剂（Cu-Ni / CZ）。香兰素（一种木质素衍生的生物油的典型化合物）的水相加氢脱氧（HDO）在促进生物质精制方面进行了研究，以研究在25 bar H 2压力和160 o C下的催化性能。所有合成的催化剂均为使用粉末XRD，拉曼光谱，H 2进行了彻底表征-TPR，HR-TEM，HAADF-STEM，EDS映射和XPS。发现与其他双金属或单金属催化剂相比，Ni / CZ（Cu-Ni / CZ-B）纳米复合材料上15 wt％的Cu活性显着增强，展现出约98％的香兰素转化率和约94％的2-选择性。甲氧基-4-甲基苯酚为所需产品。与Cu-Ni / CeO 2和Cu-Ni / ZrO 2相比，Cu-Ni / CZ-B催化剂的活性提高了约4倍。，单氧化物支持的对应物。在每个物种的界面处都有协同效应，从而解释了具有优越的催化性能和更高的稳定性，其中镍，铜和二氧化铈-氧化锆载体之间的电子相互作用产生了新的活性位点。XRD和HR‐TEM结果表明，在二氧化铈-氧化锆上形成了Cu-Ni双金属相，这有助于增强催化性能，而催化活性没有明显下降，并且对11个连续的催化循环具有所需的产物选择性，证明了其优异的稳定性和可重复性该催化剂体系。
更新日期：2018-06-13
中文翻译：
高效无贵金属铜促进镍-铈-锆-锆纳米催化剂的生物燃料升级设计
通过简单的共沉淀/浸渍方法，已经开发出了一系列新的不含贵金属的双金属负载Cu-Ni的二氧化铈-氧化锆催化剂（Cu-Ni / CZ）。香兰素（一种木质素衍生的生物油的典型化合物）的水相加氢脱氧（HDO）在促进生物质精制方面进行了研究，以研究在25 bar H 2压力和160 o C下的催化性能。所有合成的催化剂均为使用粉末XRD，拉曼光谱，H 2进行了彻底表征-TPR，HR-TEM，HAADF-STEM，EDS映射和XPS。发现与其他双金属或单金属催化剂相比，Ni / CZ（Cu-Ni / CZ-B）纳米复合材料上15 wt％的Cu活性显着增强，展现出约98％的香兰素转化率和约94％的2-选择性。甲氧基-4-甲基苯酚为所需产品。与Cu-Ni / CeO 2和Cu-Ni / ZrO 2相比，Cu-Ni / CZ-B催化剂的活性提高了约4倍。，单氧化物支持的对应物。在每个物种的界面处都有协同效应，从而解释了具有优越的催化性能和更高的稳定性，其中镍，铜和二氧化铈-氧化锆载体之间的电子相互作用产生了新的活性位点。XRD和HR‐TEM结果表明，在二氧化铈-氧化锆上形成了Cu-Ni双金属相，这有助于增强催化性能，而催化活性没有明显下降，并且对11个连续的催化循环具有所需的产物选择性，证明了其优异的稳定性和可重复性该催化剂体系。
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