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NiCo/Al_(2)O_(3)nanocatalysts for the synthesis of 5-amino-1-pentanol and 1,5-pentanediol from biomass-derived 2-hydroxytetrahydropyran

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Green Chemical Engineering 2024年第1期5卷 119-131页

作者： Jian Yang Jia Zhang Enrico Benassi Xuemei Li Hailong Liu Weiguo Fang Junying Tian chungu xia Zhiwei Huang State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China School of Petrochemical Engineering Lanzhou University of TechnologyLanzhou730050China Novosibirsk State University Novosibirsk630090Russia University of Chinese Academy of Sciences Beijing100049China

Al_(2)O_(3)-supported monometallic Ni,Co,and bimetallic Ni-Co nanocatalysts originated from layered double hydroxide precursors were synthesized by co-precipitation method,and used for the synthesis of useful 5-amino-1-pentanol(5-AP)and 1,5-pentanediol(1,5-PD)by reductive amination(RA)or direct hydrogenation of biofurfuralderived 2-hydroxytetrahydropyran(2-HTHP),*** both reactions,the yield of the target products decreased monotonously with the increasing amounts of Co in the NiCo/Al_(2)O_(3)catalysts,owing probably to the replacement of highly reactive Ni by Co component with inferior hydrogenation activity at the low reaction temperature of 60℃.However,the incorporation of Co could improve the reducibility of the NiCo/Al_(2)O_(3)bimetallic catalysts and promote the reaction stability of the catalysts,especially for Ni_(2)Co1/Al_(2)O_(3),in both reactions with over 180 h *** of the catalysts before and after the reaction showed that the incorporating Co could inhibit the sintering of metal particles and hinder the surface oxidation of the more reactive Ni0species,thanks to the formation of Ni-Co alloy in the bimetallic ***-based modeling of the reaction mechanisms is also performed,supporting the reaction pathway proposed previously and also the much higher activity of Ni in the RA of 2-HTHP as compared with Co.

关键词： NiCo bimetallic catalysts Layered double hydroxide Reductive amination Amino alcohol Quantum chemical calculations

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Natural attapulgite supported nano-Ni catalysts for the efficient reductive amination of biomass-derived aldehydes and ketones

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Green Synthesis and Catalysis 2024年第1期5卷 42-50页

作者： Jia Zhang Jian Yang Xuemei Li Bin Mu Hailong Liu chungu xia Aiqin Wang Zhiwei Huang State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Key Laboratory of Clay Mineral Applied Research of Gansu Province Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China

The efficient synthesis of useful primary amines via reductive amination of biomass-based aldehydes and ketones over earth-abundant base metal catalysts is an attractive biomass value-adding technology yet facing lots of ***,natural attapulgite(ATP)was applied as support for the fabrication of active Ni catalysts with different Ni loadings(5–30 wt%)by the deposition-precipitation *** Ni/ATP-550 catalyst with 10–15 wt%Ni loadings was found to present the highest catalytic performance for the synthesis of valuable 5-amino-1-pentanol(5-AP)via reductive amination of biofurfural-derived 2-hydroxytetrahydropyran among a variety of commonly used oxide supports loaded Ni catalysts,as well as ATP supported nickel catalysts with other loadings,achieving 5-AP yield up to 94%.The intrinsic activity of the Ni/ATP catalysts was found to depend strongly on the Ni^(0) crystallite size and Ni^(0) fraction of the catalysts,which generally increased with increasing Ni^(0) crystallite size and fraction,owing probably to the hydrogenation of imine intermediate is a structure-sensitive *** efficient 10Ni/ATP-550 catalyst also exhibited good activity and stability in the reductive amination of several other biomass-derived aldehydes and ketones to their corresponding primary amines with good to excellent yields(81%–99%).This work provided a clean and efficient natural ATP-supported non-noble metal nickel-based catalytic system for the reductive amination of aldehydes and ketones to synthesize high-value-added primary amines,which could be a promising candidate for the industrial production of amines.

关键词： Attapulgite Nano-Ni catalyst Reductive amination 5-Amino-1-pentanol Structure-activity relationship

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酚酸与蛋白质和碳水化合物相互作用及对面包面团的影响研究进展

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食品科学 2024年第9期45卷 272-282页

作者：辛嘉英刘思淼葛怿泽宋增武锁博海夏春谷哈尔滨商业大学食品科学与工程重点实验室黑龙江哈尔滨150028 中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室甘肃兰州730000

近年来,研究人员常利用食品各组分之间的相互作用调节其感官性状和功能特性。酚酸、蛋白质和碳水化合物三者在面食制品中广泛存在并发挥着重要作用。目前为止,研究主要集中在酚酸-蛋白质和酚酸-碳水化合物的相互作用,以及二者相互作用... 详细信息

近年来,研究人员常利用食品各组分之间的相互作用调节其感官性状和功能特性。酚酸、蛋白质和碳水化合物三者在面食制品中广泛存在并发挥着重要作用。目前为止,研究主要集中在酚酸-蛋白质和酚酸-碳水化合物的相互作用,以及二者相互作用在食品加工、机体保健等方面的应用。酚酸、蛋白质、碳水化合物所构成的三元体系中伴随着复杂的相互作用,这些相互作用能够赋予面食制品不同的感官性状和功能特性。本文主要介绍了酚酸、蛋白质和碳水化合物三者间的相互作用及其影响面包面团感官特性和功能特性等的研究进展,以期为酚酸、蛋白质和碳水化合物组成的三元体系在面食制品中的应用提供理论指导。

关键词：酚酸蛋白质碳水化合物相互作用三元体系

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多相催化氧化伯醇制备羧酸的研究进展

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精细化工 2024年第7期41卷 1393-1403页

作者：薛飞刘梦力廖敏李臻夏春谷王金棒中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室甘肃兰州730000 江西省烟草公司赣州市公司江西赣州341000 中国烟草总公司郑州烟草研究院河南郑州450001

伯醇催化氧化制羧酸是有机合成中极为重要的转化过程,具有广泛的应用前景。对于多相催化体系,高效催化剂的制备一直是研究的热点和难点。该文对近年来涉及多相催化氧化伯醇制备羧酸的文献进行了全面的梳理。从单金属及其氧化物和双金属... 详细信息

伯醇催化氧化制羧酸是有机合成中极为重要的转化过程,具有广泛的应用前景。对于多相催化体系,高效催化剂的制备一直是研究的热点和难点。该文对近年来涉及多相催化氧化伯醇制备羧酸的文献进行了全面的梳理。从单金属及其氧化物和双金属及其氧化物基催化剂,以及是否采用载体等角度系统评估了伯醇氧化多相催化剂的发展现状和趋势;介绍了杂多酸催化和绿色催化的研究进展;展望了多相催化在工业应用中的发展前景和挑战。

关键词：伯醇催化氧化多相催化羧酸金属催化剂金属氧化物催化剂

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利用一碳资源生产单细胞蛋白在饲料中的应用研究进展

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饲料工业 2024年第8期45卷 32-43页

作者：贺姣辛嘉英张卫丹徐景懿夏春谷哈尔滨商业大学食品科学与工程重点实验室哈尔滨商业大学黑龙江哈尔滨150076 中国科学院兰州物理化学研究所羰基合成与选择氧化国家重点实验室甘肃兰州730000

随着全球温室气体排放量的持续增加以及出现饲料资源短缺的新趋势,某些微生物利用甲烷(CH_(4))、二氧化碳(CO_(2))、一氧化碳(CO)和甲醇(CH_(3)OH)等一碳资源为底物发酵生产单细胞蛋白(Single cell protein,SCP),这种营养丰富,可持续生... 详细信息

随着全球温室气体排放量的持续增加以及出现饲料资源短缺的新趋势,某些微生物利用甲烷(CH_(4))、二氧化碳(CO_(2))、一氧化碳(CO)和甲醇(CH_(3)OH)等一碳资源为底物发酵生产单细胞蛋白(Single cell protein,SCP),这种营养丰富,可持续生产的新型高质量蛋白是未来饲料蛋白替代的新趋势。此外,单细胞蛋白具有生产周期短、生产效率高、原料资源丰富且容易获得、营养价值高等优点,可大规模工业化生产,在减缓温室效应中发挥重要作用。根据其氨基酸组成,可以作为动物蛋白饲料的替代来源。文章主要介绍了一碳资源经微生物转化为单细胞蛋白及其在饲料应用中的研究进展,分析单细胞蛋白商业化生产面临的挑战及未来解决措施,最后展望了单细胞蛋白在粮食安全和碳减排的双重需求下潜在应用价值。

关键词：一碳资源微生物单细胞蛋白饲料应用碳减排

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电感耦合等离子体质谱仪在线稀释进样系统设计及其便捷测定氢甲酰化反应液中钴和磷元素

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分析测试技术与仪器 2024年第4期30卷 209-214页

作者：曾波刘祺壬王国峰郧栋许传芝李臻夏春谷中国科学院兰州化学物理研究所甘肃兰州730000

为了快速测定氢甲酰化反应有机相中钴和磷元素的浓度,对电感耦合等离子体质谱仪(ICP-MS)进样系统进行改造,实现直接对有机相进行分析.使用反应溶剂对待测物料进行在线自动稀释,然后直接进样测试元素的含量.样品的稀释倍数由进样泵参数... 详细信息

为了快速测定氢甲酰化反应有机相中钴和磷元素的浓度,对电感耦合等离子体质谱仪(ICP-MS)进样系统进行改造,实现直接对有机相进行分析.使用反应溶剂对待测物料进行在线自动稀释,然后直接进样测试元素的含量.样品的稀释倍数由进样泵参数进行校准,测试结果与手动稀释的误差低于3%.改进后的ICP-MS可以及时监测氢甲酰化反应过程中钴和磷浓度,发现实际生产过程中产能不足的问题,进一步指导促进增产的具体应对方案.

关键词：电感耦合等离子体质谱仪氢甲酰化反应在线稀释便捷测试有机相进样

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Bioinspired manganese complexes catalyzed epoxidation for the synthesis of the epoxyketone fragment of carfilzomib

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Chinese Chemical Letters 2019年第3期30卷 698-701页

作者： Bin Qiu chungu xia Wei Sun Key Laboratory for Oxo Synthesis and Selective Oxidation Suzhou Research Institute of LICP Lanzhou Institute of Chemical Physics (LICP) Chinese Academy of Sciences University of Chinese Academy of Sciences

We report herein an efficient catalytic epoxidation reaction for the synthesis of epoxyketone(tert-butyl((S)-4-methyl-1-((R)-2-methyloxiran-2-yl)-1-oxopentan-2-yl)carbamate), which is an important synthetic intermediate of carfilzomib. A series of bioinspired manganese complexes bearing N4 ligands are carefully investigated in the epoxidation of enone precursor with H_2O_2 as oxidant in the presence of carboxylic acid(e.g., acetic acid).

关键词： Catalytic epoxidation Bioinspired manganese complexes Hydrogen peroxide Epoxyketone Carfilzomib

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Versatile MOF-derived cobalt catalyst for the reductive amination

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Science China Materials 2017年第12期60卷 1269-1271页

作者： Haihong Wu Chaoren Shen chungu xia Lin He State Key Laboratory for Oxo Synthesis and Selective Oxidation Suzhou Research Institute of LICP Lanzhou Institute of Chemical Physics (LICP) Chinese Academy of Sciences Lanzhou 730000 China University of Chinese Academy of Sciences Beijing 100049 China

The tunable metal center and the tailorable organic linker of metal-organic framework(MOF)make the characteristic of ultrahigh porosity,controllable pore size,crystalline nature and highly-ordered structures[1].Since its emergence[2,3],it represents one of the most celebrated functional *** to the rich diversity of MOF family,a vast of important applications including the storage of gas,recognition of molecules as well as

关键词： DABCO Co NH MOF TPA

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Biosynthesis of poly-3-hydroxybutyrate with a high molecular weight by methanotroph from methane and methanol

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Journal of Natural Gas Chemistry 2008年第1期17卷 103-109页

作者： Yingxin Zhang Jiaying Xin Linlin Chen Hao Song chungu xia State Key Laboratory for Oxo Synthesis ＆ Selective Oxidation Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Lanzhou 730000 China College of Food Engineering Harbin University of Commerce Harbin 150076 China Graduate University of Chinese Academy of Sciences Beijing 10039 China

Poly-3-hydroxybutyrate （PHB） can be produced by various species of bacteria. Among the possible carbon sources, both methane and methanol could be a suitable substrate for the production of PHB. Methane is cheap and plentiful not only as natural gas, but also as biogas. Methanol can also maintain methanotrophic activity in some conditions. The methanotrophic strain Methylosinus trichosporium IMV3011 can accumulate PHB with methane and methanol in a brief nonsterile process. Liquid methanol （0.1%） was added to improve the oxidization of methane. The studies were carried out using shake flasks. Cultivation was performed in two stages： a continuous growth phase and a PHB accumulation phase under the conditions short of essential nutrients （ammonium, nitrate, phosphorus, copper, iron （Ⅲ）, magnesium or ethylenediamine tetraacetate （EDTA）） in batch culture. It was found that the most suitable growth time for the cell is 144 h. Then an optimized culture condition for second stage was determined, in which the PHB concentration could be much increased to 0.6 g/L. In order to increase PHB content, citric acid was added as an inhibitor of tricarboxylic acid cycle （TCA）. It was found that citric acid is favorable for the PHB accumulation, and the PHB yield was increased to 40% （w/w） from the initial yield of 12% （w/w） after nutrient deficiency cultivation. The PHB produced is of very high quality with molecular weight up to 1.5 × 10^6Da.

关键词： poly-3-hydroxybutyrate methanotrophs methane methanol cultivation biosynthesis high molecular weight

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Chemical equilibrium controlled synthesis of polyoxymethylene dimethyl ethers over sulfated titania

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Journal of Energy Chemistry 2015年第2期24卷 239-244页

作者： Huaju Li Huanling Song Feng Zhao Liwei Chen chungu xia Laboratory for Nano-Catalytic Material & Technology Division of Advanced Nano?materials Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of Sciences State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics Chinese Academy of Sciences i-Lab Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences

The chemical equilibrium and reaction kinetic behavior in the synthesis of polyoxymethylene dimethyl ethers （DMMn） were investigated over sulfated titania in order to reveal the decisive factor controlling the reaction. The results showed that the molar ratio of adjacent DMMn products in equilibrium solution had the same value, which depended absolutely on the reaction temperature. Meanwhile, the reactions had the same DMMn products distributions under varied reaction conditions. The equilibrium constants of the related step-wise reactions for DMMn formation were equal, which were calculated based on the bulk compositions of the reaction solution. And thus, the selectivity to DMMn was mainly controlled by the chemical equilibrium, i.e., thermodynamic control. In brief, the present results provide some guidance for future synthesis of DMMn.

关键词： polyoxymethylene dimethyl ethers sulfated titania chemical equilibrium reaction kinetic molar ratio

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