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Vicinal hydroxyl group-inspired selective oxidation of glycerol to glyceric acid on hydroxyapatite supported Pd catalyst

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Green Energy & Environment 2022年第4期7卷 691-703页

作者： Difan Li xiuge zhao Qingqing Zhou Bingjie Ding Anna Zheng Qingpo Peng Zhenshan Hou Key Laboratory for Advanced Materials Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China

Selective oxidation of glycerol provides a feasible route towards the sustainable synthesis of high value-added ***,the hydroxyapatite(HAP)supported palladium(Pd)species were fabricated by impregnation and subsequent *** as-obtained heterogeneous Pd catalyst afforded not only excellent selectivity to glyceric acid(GLA)up to 90%with 59%conversion of glycerol but also good recyclability by using molecular oxygen as an oxidant under mild *** characterization of catalysts indicated that both the surface basicity and Pd sites on the catalyst played a crucial role in promoting glycerol ***,it demonstrated that the presence of the vicinal hydroxyl group of glycerol molecule can assist the oxidation reaction via forming a coordination between the vicinal hydroxyl group and Ca^(2+) sites on HAP-derived *** this catalytic process,the secondary hydroxyl of glycerol kept untouched and the primary hydroxyl of glycerol was converted into carboxyl group,while the Pd species acted as active centers for cooperatively promoting the subsequent oxidation to generate ***,this catalytic system can be extended widely for the oxidative conversion of other vicinal diols into the corresponding a-hydroxycarboxylic acids *** labeling experiment using H_(2)^(18)O confirmed that H_(2)O not only acted as solvent but also was involved in the catalytic *** the basis of the results,a possible reaction mechanism has been *** HAP-supported Pd catalytic system has been shown to serve as an effective approach for the upgrading of bio-derived vicinal diols to high value-added chemicals.

关键词： Hydroxyapatite Palladium Glycerol oxidation Glyceric acid Vicinal hydroxyl group

Catalytic transfer hydrogenolysis of C–O bonds in lignin model compounds without arene hydrogenation

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Green Chemical Engineering 2022年第1期3卷 25-33页

作者： Kai Cui xiuge zhao Qingpo Peng Honghui Gong Xinjia Wei Jiajia Wang Manyu Chen Zhenshan Hou Key Laboratory for Advanced Materials Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China

The shortage of resources and the destruction of the environment have caused serious resource and environmental problems shared by all countries around the world. As a ubiquitous renewable resource, biomass has great prospects for replacing fossil energy and attracted attention from the society. The use of catalytic approach to transform biomass into high-value chemicals is an effective way to use biomass efficiently. In this work, Nisupported catalysts has been developed for the selective cleavage of C–O bonds in lignin model compounds with 2-propanol as the hydrogen source solvent. Among these catalysts, it was indicated that zirconium phosphate(Zr P)-supported Ni catalysts were highly efficient and recyclable for alkyl-aryl ether(α-O-4 and β-O-4) cleavage in lignin model compounds. The further investigation demonstrated that the transfer hydrogenolysis of the C–O bond is highly selective, which afforded phenols and aromatics as dominant products without the products arising from hydrogenation of aromatic rings. Through a series of characterization of the catalyst, it was demonstrated that the medium strong acid sites of the Zr P support promoted the cleavage of alkyl-aryl ethers(α-O-4 and β-O-4),and Br?nsted acid sites favored for achieving high selectivity toward C–O bond cleavage. Additionally, Ni(0) sites on the Zr P catalysts were responsible for the catalytic transfer hydrogenolysis.

关键词： C–O bond cleavage Hydrogenolysis Zirconium phosphate Biomass conversion Ni catalysts

Catalytic hydrogenation of aromatic nitro compounds by functionalized ionic liquids-stabilized nickel nanoparticles in aqueous phase:The influence of anions

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Science China Chemistry 2010年第7期53卷 1541-1548页

作者： HU Yu YU YinYin zhao xiuge YANG HanMing FENG Bo LI Huan QIAO YunXiang HUA Li PAN ZhenYan HOU ZhenShan Key Laboratory for Advanced Materials Research Institute of Industrial CatalysisEast China University of Science and TechnologyShanghai 200237China Key Laboratory of Catalysis and Materials Science of the State Ethnic Affairs Commission Ministry of EducationSouth-Central University for NationalitiesWuhan 430074China

Two kinds of nickel nanoparticles (NPs) well-dispersed in aqueous phase have been conveniently prepared by reducing nickel(II) salt with hydrazine in the presence of amino group (-NH2) functionalized ionic liquids:1-(3-aminopropyl)-2,3-dimethylimidazolium bromide ([AMMIM][Br]) and 1-(3-aminopropyl)-2,3-dimethylimidazolium acetate ([AMMIM][AcO]).The Ni(0) particles are composed of smaller ones which assemble in a blackberry-like *** Ni nanoparticles stabilized with [AMMIM][AcO] are much larger than those stabilized with [AMMIM][Br],and the former unexpectedly give much higher activity in the selective hydrogenation of citral and nitrobenzene (NB) in aqueous *** Ni(0) nanocatalysts dispersed in aqueous phase are stable enough to be reused at least five times without significant loss of catalytic activity and selectivity during the catalytic recycles.

关键词： functionalized ionic liquid nickel nanoparticles aqueous phase selective hydrogenation

Selective Oxidation of Glycerol with Hydrogen Peroxide Using Silica- Encapsulated Heteropolyacid Catalyst

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物理化学学报 2018年第8期34卷 886-895页

作者： YUAN Mingming LI Difan zhao xiuge MA Wenbao KONG Kang NI Wenxiu GU Qingwen HOU Zhenshan Key Laboratory for Advanced Materials Research Institute of Industrial Catalysis School of Chemistry & Molecular Engineering East China University of Science and Technology Shanghai 200237 P. R. China.

The Keggin type heteropolyacids (HPAs) have attracted increasing attention due to their strong Bronsted acidity and excellent redox properties, which could play an important role in accelerating the conversion of bio-derived molecules. In this work, heteropolyacid (HPA, H_4PMo_(11)VO_(40)) encapsulated by silica was synthesized by a sol-gel method and a sequential silylation technique (HPA@SiO_2-N_2-S). The as-synthesized material was characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), scanning electron microscope (SEM) and transmission electron microscopy (TEM). The FT-IR spectra show that the HPA anions preserved their Keggin structure when incorporated into the catalyst. The XRD patterns show that HPA molecules are uniformly dispersed within the silica network. The SEM and TEM images confirm that the catalyst was composed of spherical nanometer-sized particles. The porous properties of the catalysts measured by the N_2 adsorption-desorption isotherms indicate that the Brunauer, Emmett and Teller (BET) surface area of pure SiO_2 was 287 m~2·g~(–1), but upon encapsulation of HPA into the silica matrix, a lower surface area (245 m~2·g~(–1)) was measured for the resulting material. In addition, the pore diameter was reduced after silylation. Furthermore, the hydrophobicity of the catalysts was investigated by the measurement of contact angle (CA) with water. The SiO_2 and SiO_2/HPA catalysts were completely hydrophilic and the contact angle was close to 0°. However, the contact angle of the silylated catalyst was determined to be 137°, indicating that the silylation procedure significantly increased the hydrophobicity of the catalyst. The as-prepared catalysts were also used as heterogeneous catalysts for the selective oxidation of glycerol. The prepared material exhibited excellent catalytic activity towards glycerol oxidation, in which the glycerol can be selectively transformed into formic ac

关键词：杂多酸化学分析二氧化硅合成方法

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双组分过渡金属氮化物催化剂Ⅱ.催化性能

催化学报 2000年第4期21卷 305-308页

作者：魏昭彬赵秀阁辛勤中国科学院大连化学物理研究所催化基础国家重点实验室大连116023

对共沉淀法和浸渍法制备的双组分金属氮化物催化剂MMoNx(M =Ti,Co ,Ce ,Zr ,La) ,在中压微反装置上进行了吡碇加氢脱氮、噻吩加氢脱硫、环己烯加氢及苯加氢反应性能考察 .结果表明 ,不同的金属元素和制备方法对催化剂催化性能的影响有... 详细信息

对共沉淀法和浸渍法制备的双组分金属氮化物催化剂MMoNx(M =Ti,Co ,Ce ,Zr ,La) ,在中压微反装置上进行了吡碇加氢脱氮、噻吩加氢脱硫、环己烯加氢及苯加氢反应性能考察 .结果表明 ,不同的金属元素和制备方法对催化剂催化性能的影响有很大不同 .其中 ,CoMoNx 催化剂在上述几种反应中均表现出优异的催化性能 .另外 ,共沉淀法制备的双组分金属氮化物催化剂要比浸渍法制备的催化剂活性高 .

关键词：双金属氮化物钼催化剂催化剂催化性能

α-Al_2O_3的性质对负载钯催化剂催化CO偶联反应的影响

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催化学报 2006年第10期27卷 911-915页

作者：林茜赵秀阁毕伟肖文德华东理工大学联合化学反应工程研究所上海200237

以不同来源的-αAl2O3为载体制备了用于催化CO偶联制草酸二甲酯反应的Pd/-αAl2O3催化剂,利用X射线衍射、N2吸附和X射线能谱等手段对载体进行了表征.结果表明,催化剂活性与载体的比表面积没有必然联系,但依赖于载体孔容及孔径的分布范围... 详细信息

以不同来源的-αAl2O3为载体制备了用于催化CO偶联制草酸二甲酯反应的Pd/-αAl2O3催化剂,利用X射线衍射、N2吸附和X射线能谱等手段对载体进行了表征.结果表明,催化剂活性与载体的比表面积没有必然联系,但依赖于载体孔容及孔径的分布范围.同时-αAl2O3的纯度和杂质种类对催化剂活性也有影响,少量钠氧化物和-γAl2O3的存在会大大降低催化剂的活性.此外,利用CO化学吸附法分析了催化剂活性组分的分布情况.结果表明,催化剂表面活性金属Pd的分散度达到3.94%以上时,分散度的进一步增大对CO偶联反应没有明显影响.

关键词：一氧化碳偶联亚硝酸甲酯草酸二甲酯钯氧化铝载体负载型催化剂

Contribution of Temperature Increase to Restrain the Transmission of COVID-19

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The Innovation 2021年第1期2卷 74-81页

作者： Mengyuan Ren Rongjuan Pei Bahabaike Jiangtulu Junxi Chen Tao Xue Guofeng Shen Xiaoru Yuan Kexin Li Changxin Lan Zhen Chen Xinwen Chen Yun Wang Xiaoqian Jia Zewu Li Audil Rashid Tippawan Prapamontol xiuge zhao zhaomin Dong Yali Zhang Le Zhang Rongwei Ye Zhiwen Li Wuxiang Guan Bin Wang Institute of Reproductive and Child Health Peking University/Key Laboratory of Reproductive HealthNational Health Commission of the People's Republic of ChinaBeijing 100191P.R.China Department of Epidemiology and Biostatistics School of Public HealthPeking UniversityBeijing 100191P.R.China Wuhan Institute of Virology Center for Biosafety Mega-ScienceChinese Academy of SciencesWuhanHubeiChina College of Urban and Environmental Sciences Peking UniversityBeijing 100871P.R.China Key Laboratory of Machine Perception(Ministry of Education) and School of EECSPeking UniversityBeijingChina Institute of Geographic Sciences and Natural Resources Research CASBeijing 100101P.R.China Faculty of Science Botany DepartmentUniversity of GujratHafiz Hayat CampusGujrat-50700Pakistan Research Institute for Health Sciences Chiang Mai UniversityChiang Mai 50200Thailand State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012P.R.China Beijing Advanced Innovation Center for Big Data-Based Precision Medicine Beihang UniversityBeijing 100191China

The COVID-19 outbreak has already become a global pandemic and containing this rapid worldwide transmission is of great *** impacts of temperature and humidity on the COVID-19 transmission rate are still under ***,we elucidated these relationships by utilizing two unique scenarios,repeated measurement and natural experiment,using the COVID-19 cases reported from January 23–February 21,2020,in *** modeling results revealed that higher temperature was most strongly associated with decreased COVID-19 transmission at a lag time of 8 *** humidity(RH)appeared to have only a slight *** findings were verified by assessing SARSCoV-2 infectivity under the relevant conditions of temperature(4C–37C)and RH(>40%).We concluded that temperature increase made an important,but not determined,contribution to restrain the COVID19 outbreak in *** suggests that the emphasis of other effective controlling polices should be strictly implemented to restrain COVID19 transmission in cold seasons.

关键词： restrain humidity COV

SO_2对Co_3O_4/Al_2O_3选择性催化氧化NO的影响

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催化学报 2000年第3期21卷 239-242页

作者：赵秀阁王辉肖文德王军华东理工大学联合化学反应工程研究所上海200237

采用流动态原位IR ,TPD及XPS技术研究了NO及SO2 在Co3 O4 /Al2 O3 金属氧化物催化剂表面上的吸附及脱附行为 ,并与该催化剂上模拟烟道气中NO的选择性催化氧化活性相关联 ,考察了SO2 对该反应过程的影响及作用机理 .

关键词：氧化钴氧化铝一氧化氮催化氧化二氧化硫

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双组分过渡金属氮化物催化剂Ⅰ.制备和表征

催化学报 2000年第3期21卷 225-228页

作者：魏昭彬赵秀阁辛勤中国科学院大连化学物理研究所催化基础国家重点实验室大连116023

用共沉淀法和浸渍法制备了以Mo为主并含有少量金属Ti,Zr,Co ,Ce或La的双组分氮化物 ,利用XRD ,BET和DTA表征了样品的物相组成、孔结构和氮化过程 .结果表明 ,在共沉淀法制备的样品上 ,Co或Zr可以和Mo生成某种无定形复合氮化物CoMoNx 或Z... 详细信息

用共沉淀法和浸渍法制备了以Mo为主并含有少量金属Ti,Zr,Co ,Ce或La的双组分氮化物 ,利用XRD ,BET和DTA表征了样品的物相组成、孔结构和氮化过程 .结果表明 ,在共沉淀法制备的样品上 ,Co或Zr可以和Mo生成某种无定形复合氮化物CoMoNx 或ZrMoNx;Ti和Mo生成TiN Mo2 N混合物 ;稀土元素Ce或La的钼酸盐不能被氮化 .对于用共沉淀法制备的样品 ,第二组分的加入有利于Mo的氮化 .浸渍法制备的样品上除Mo2 N外 ,还有MoO2 相存在 .不同的制备方法对氮化物的比表面积也有影响 .

关键词：钼催化剂制备共沉淀法浸清法双金属氮化物