葡萄糖氧化制葡萄糖酸的催化剂结构敏感性研究进展

doi:10.1016/S1872-2067(20)63590-2

催化学报 ›› 2020, Vol. 41 ›› Issue (9): 1320-1336.DOI: 10.1016/S1872-2067(20)63590-2

葡萄糖氧化制葡萄糖酸的催化剂结构敏感性研究进展

严文娟^a, 张东培^a, 孙玉^a, 周子淇^a, 杜屹航^a, 杜一垚^a, 李玉姗^a, 刘梦媛^a, 张玉明^b, 沈健^c, 金鑫^a

a 中国石油大学(华东)化学工程实验教学中心, 重质油加工国家重点实验室, 山东青岛 266580, 中国;
b 中国石油大学(北京)工艺流体过滤和分离北京重点实验室, 重质油加工国家重点实验室, 北京 102249, 中国;
c 太平洋西北国家实验室物理科学部, 华盛顿州里奇兰市 99354, 美国

收稿日期:2020-01-16 修回日期:2020-02-27 出版日期:2020-09-18 发布日期:2020-08-08
通讯作者: 金鑫
基金资助:
国家自然科学基金（21706290）；山东省自然科学基金（ZR2017MB004，ZR2017BB007）；山东省博士后创新项目（201703016）；青岛市博士后资助项目（BY20170210）；青岛市源头创新项目（17-1-1-67-jch，17-1-1-80-jch）；中央高校基本科研业务费专项资助（18CX02145A，17CX02017A）；中国石油大学教师科研启动经费（YJ201601058）.

Structural sensitivity of heterogeneous catalysts for sustainable chemical synthesis of gluconic acid from glucose

Wenjuan Yan^a, Dongpei Zhang^a, Yu Sun^a, Ziqi Zhou^a, Yihang Du^a, Yiyao Du^a, Yushan Li^a, Mengyuan Liu^a, Yuming Zhang^b, Jian Shen^c, Xin Jin^a

a State Key Laboratory of Heavy Oil Processing, Center for Chemical Engineering Experimental Teaching, China University of Petroleum(East China), Qingdao 266580, Shandong, China;
b State Key Laboratory of Heavy Oil Processing, Beijing Key Laboratory of Process Fluid Filtration and Separation, China University of Petroleum(Beijing), Beijing 102249, China;
c Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA, 99354, USA

Received:2020-01-16 Revised:2020-02-27 Online:2020-09-18 Published:2020-08-08
Supported by:
This study was supported by the National Natural Science Foundation (21706290), Natural Science Foundation of Shandong Province (ZR2017MB004, ZR2017BB007), Postdoctoral Research Funding of Shandong Province (201703016), Qingdao Postdoctoral Research Funding (BY20170210), Fundamental Research Funding of Qingdao (17-1-1-67-jch, 17-1-1-80-jch), "Fundamental Research Funds for the Central Universities" (18CX02145A, 17CX02017A) and new faculty start-up funding from the China University of Petroleum (YJ201601058).

摘要/Abstract

摘要： 葡萄糖酸及其衍生物已广泛应用于食品和医药加工生产工业，学术界和工业界对葡萄糖酸的绿色合成非常关注.目前，在工业上采用葡萄糖发酵法来制备葡萄糖酸.尽管经过多年的研究和技术改进，该工艺仍然存在很多问题，诸如废水处理能耗高、酶分离程序复杂等技术难题.因此，开发适应时代发展的高环保和低污染等要求的新工艺方法迫在眉睫.近年来，非均相催化剂已成功应用于催化氧化反应.在葡萄糖催化氧化制葡萄糖酸工艺中，Au，Pt，Pd固载催化剂因展现出优异的性能而被广泛的研究报道.由Au，Pt，Pd等贵金属的双金属催化剂也展现出了更高的活性，因此采用非贵金属作为第二种金属也可降低催化剂成本.在过去十几年中，研究人员致力于探索合成方法/条件、催化剂结构、反应条件等因素对催化剂性能的影响规律，并归纳出葡萄糖氧化得到葡萄糖酸的反应机理，最终寻找到进一步提高催化剂活性和葡萄糖酸的选择性、以及延长催化剂生命周期的科学方法.
在诸多研究成果报道中，催化剂粒径普遍被认为是影响葡萄糖氧化反应速率的最主要因素之一.改变合成方法和条件可调控催化剂粒径，如合成方法、配位体种类、合成条件等.本文详细讨论了影响催化剂理化性能的几个因素：（1）在葡萄糖氧化为葡萄糖酸反应过程中，碱性添加剂可以调节反应溶液的pH值，进而调控催化剂性能.但是碱的添加不但造成反应设备的腐蚀，也容易导致催化剂失活，提高了催化剂再生成本.因此，开发出在酸性条件中仍然能展现出高性能的催化剂非常有必要.（2）由于氧气在反应溶液中溶解度较低，限制了产物的收率的提高，因此采用过氧化氢很有可能替代氧气用于葡萄糖氧化过程.（3）减少活性位在催化剂表面的密度，并提高金属活性位在催化剂表面的分散度，可以有效的缓解因催化剂活性位中毒、颗粒烧结、金属浸出、有机物吸附等诸多原因造成的催化剂失活现象.因此进一步研究催化剂合成方法来获得高分散的金属催化剂是非常有必要的.（4）在添加碱和不添加碱的条件下葡萄糖氧化制葡萄糖酸反应的机制是不同的，所以深入研究反应动力学和反应机理，对于催化工艺的开发都具有重大意义.（5）工艺操作条件对葡萄糖酸产率具有显著影响，葡萄糖氧化包含了众多连续-平行反应，生成众多副主产物，因此要弄清楚反应条件对葡萄糖酸产率的影响机制，需要系统和全面的研究.（6）贵金属储量低和价格高等因素进一步限制了提高该工艺方法的经济收益，因此，开发出非贵金属基催化氧化葡萄糖氧化的工艺方法是潜在的重要研究目标和方向.
总之，本综述总结了最近5年来非均相催化剂在葡萄糖氧化制葡萄糖酸反应中最新进展，主要讨论了金、铂和钯基的单金属和双金属催化剂性能，同时辅以其他金属催化剂，提出了葡萄糖氧化制葡萄糖酸绿色合成方法的未来机遇和挑战，以期为设计出有效的非均相催化剂，用于催化氧化生物质及其衍生物的反应中.

关键词: 葡萄糖, 葡萄糖二酸, 贵金属, 氧化, 非均相催化剂

Abstract: Gluconic acid and its derivatives have been widely used in the food and pharmaceutical industries. Conventional processes that involve the conversion of glucose into gluconic acid via fermentation present several technological shortcomings as they involve energy-intensive wastewater treatment and complex enzyme separation. Greener oxidation processes over heterogeneous metal catalysts have attracted increasing attention worldwide. Au-, Pt- and Pd-based heterogeneous catalysts have been extensively used for the chemical oxidation of glucose to gluconic acid. Bimetallic catalysts synthesized by adding either noble or inexpensive metals have also presented excellent performance for the oxidations of glucose. In particular, particle size, which has been recognized as the most important factor that affect catalytic performances, could be rationally tuned by changing the types of support and ligand as well as the synthesis conditions. In this perspective review, we summarize and critically discuss the recent advances in the structural design of mono- and bimetallic catalysts for the oxidation of glucose in aqueous media. Furthermore, the challenges of developing catalysts for the green synthesis of gluconic acid have been highlighted. This review provides alternative insights for designing effective catalytic materials for the catalytic oxidation of bio-derived oxygenates over heterogeneous catalysts.

Key words: Glucose, Gluconic acid, Noble metal, Oxidation, Heterogeneous catalyst

严文娟, 张东培, 孙玉, 周子淇, 杜屹航, 杜一垚, 李玉姗, 刘梦媛, 张玉明, 沈健, 金鑫. 葡萄糖氧化制葡萄糖酸的催化剂结构敏感性研究进展[J]. 催化学报, 2020, 41(9): 1320-1336.

Wenjuan Yan, Dongpei Zhang, Yu Sun, Ziqi Zhou, Yihang Du, Yiyao Du, Yushan Li, Mengyuan Liu, Yuming Zhang, Jian Shen, Xin Jin. Structural sensitivity of heterogeneous catalysts for sustainable chemical synthesis of gluconic acid from glucose[J]. Chinese Journal of Catalysis, 2020, 41(9): 1320-1336.

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葡萄糖氧化制葡萄糖酸的催化剂结构敏感性研究进展

Structural sensitivity of heterogeneous catalysts for sustainable chemical synthesis of gluconic acid from glucose

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