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Subnanometric bimetallic Pt–Pd clusters in zeolites for efficient hydrogen production and selective tandem hydrogenation of nitroarenes

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Science China Chemistry 2024年第9期67卷 2911-2917页

作者： Jiafu Li Tao Cai Yanran Feng Xia Liu Ning Wang qiming sun Institute of Sustainable Energy and Resources College of Chemistry and Chemical Engineering Key Laboratory of Shandong Provincial Universities for Functional Molecules and Materials Qingdao University Innovation Center for Chemical Sciences College of Chemistry Chemical Engineering and Materials Science Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University

The solvolysis of ammonia borane（AB） and the hydrogenation of nitroarenes represent significant reactions for hydrogen generation and value-added chemical synthesis. The strategic engineering of the catalysts is imperative for surmounting obstacles associated with their stability and catalytic efficiency. In this work, subnanometric bimetallic Pt–Pd clusters were encapsulated within silicalite-1（S-1） zeolites through a ligand-protected in-situ hydrothermal synthesis method. The synergetic effect of bimetallic composition and zeolite confinement markedly enhances the catalytic performance of representative Pt0.5Pd0.5@S-1-H catalyst, affording exceptional turnover frequency（TOF） values of 1,043 and 573 molH2molmetal-1min-1for AB hydrolysis and methanolysis at ambient conditions, respectively, surpassing most of the state-of-the-art Pt-based *** and isotopic experiments reveal that the bimetallic catalytic system remarkably boosts the O–H cleavage of water,thereby facilitating the H2production from AB hydrolysis. Remarkably, a conspicuous synergistic effect is demonstrated in the shape-selective tandem hydrogenation of nitroarenes, with the bimetallic catalyst facilitating both AB hydrolysis and nitroarene hydrogenation, giving a high TOF value of 1,260 h-1under atmospheric pressure. This study not only demonstrates the effectiveness of bimetallic nanocatalysts encapsulated in zeolites for hydrogen production from chemical hydrogen storage materials, but also paves the way for the design of catalysts with multifunctional active sites capable of synergistically promoting tandem catalytic processes.

关键词： subnanometer bimetallic cluster zeolite synergistic effect ammonia borane solvolysis selective tandem hydrogenation

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山东北部泥质海岸带白浪河地区地下水水化学演化过程

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海洋地质前沿 2024年第3期40卷 64-74页

作者：常新月高茂生罗锡明孙启明刘震林侯国华中国地质调查局青岛海洋地质研究所青岛266237 中国地质大学(北京)海洋学院北京100083

莱州湾沿岸是中国海(咸)水入侵典型区域之一,受多次海侵海退事件影响,形成了复杂的地下含水系统。为探究其地下水系统水化学特征及演化规律,对比分析白浪河地区内地下水的水化学特征及主要离子的变化规律,研究了不同分区的水化学演化过... 详细信息

莱州湾沿岸是中国海(咸)水入侵典型区域之一,受多次海侵海退事件影响,形成了复杂的地下含水系统。为探究其地下水系统水化学特征及演化规律,对比分析白浪河地区内地下水的水化学特征及主要离子的变化规律,研究了不同分区的水化学演化过程。结果表明,内陆的咸水主要由淡水/卤水混合形成,滨海的咸水主要由淡水/海水混合形成。现存卤水在形成过程中发生了淡水的混入,水岩相互作用和阳离子交换在一定程度上改变了卤水的水化学组成。矿物饱和指数结果表明,不同分区的地下水体中,方解石和白云石基本处于饱和状态,岩盐均未达到饱和状态,石膏仅在卤水中达到饱和状态。从陆到海,地下水系统中发生的阳离子交换过程不同,淡水区和微咸水区浅层的地下水主要是水中的Ca^(2+)与含水介质吸附的Na^(+)交换,而其他分区的阳离子交换过程与之相反。

关键词：白浪河演化过程卤水矿物饱和指数

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Zeolite-encaged Ultrasmall Pt-Zn Species with Trace Amount of Pt for Efficient Propane Dehydrogenation

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Chemical Research in Chinese Universities 2023年第6期39卷 870-876页

作者： QU Ziqiang ZHANG Tianjun YIN Xichen ZHANG Junyi XIONG Xiaoyun sun qiming Innovation Center for Chemical Science College of ChemistryChemical Engineering and Materials ScienceJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123P.R.China College of Chemistry and Materials Science Hebei UniversityBaoding 071002P.R.China PetroChina Lanzhou Petrochemical Company Lanzhou 730000P.R.China Lanzhou Petrochemical Research Center Petrochemical Research InstitutePetroChinaLanzhou 730000P.R.China

Propane dehydrogenation(PDH)has become a globe-welcoming technology to meet the massive demand for propylene,but the most commonly used Pt-based catalysts suffer from quick sintering,poor selectivity for propylene,and unsatisfied Pt ***,a series of Silicalite-1(S-1)zeolite-encaged ultrasmall Pt-Zn clusters with a trace amount of Pt[40—180 ppm(parts per million)]were developed by using a one-pot ligand-protected direct H_(2) reduction ***,the extremely low amount of Pt can significantly promote the activity of zeolite-encaged Zn catalysts in PDH *** to the high Pt dispersion,the synergy between Pt and Zn species,and the confinement effect of zeolites,the optimized PtZn@S-1 catalyst with 180 ppm Pt and 1.88%(mass fraction)Zn,exhibited an extraordinarily high propane conversion(33.9%)and propylene selectivity(99.5%)at 550℃with a weight hourly space velocity(WHSV)of 8 h^(-1),affording an extremely high propylene formation rate of 340.7 mol_(C_(3)H_(6))·g_(Pt^(-1))·h^(-1).This work provides a reference for the preparation of zeolite-encaged metal catalysts with high activity and noble metal utilization in PDH reactions.

关键词： Propane dehydrogenation Zeolite Confinement effect Bimetallic catalyst Pt-Zn

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Deep Learning Based Data Fusion for Sensor Fault Diagnosis and Tolerance in Autonomous Vehicles

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Chinese Journal of Mechanical Engineering 2021年第3期34卷 158-168页

作者： Huihui Pan Weichao sun qiming sun Huijun Gao Research Institute of Intelligent Control and Systems Harbin Institute of TechnologyHarbin 150001China The Ningbo Institute of Intelligent Equipment Technology Co. LtdNingbo 315200China

Environmental perception is one of the key technologies to realize autonomous *** vehicles are often equipped with multiple sensors to form a multi-source environmental perception *** sensors are very sensitive to light or background conditions,which will introduce a variety of global and local fault signals that bring great safety risks to autonomous driving system during long-term *** this paper,a real-time data fusion network with fault diagnosis and fault tolerance mechanism is *** introducing prior features to realize the lightweight network,the features of the input data can be extracted in real time.A new sensor reliability evaluation method is proposed by calculating the global and local confidence of *** the temporal and spatial correlation between sensor data,the sensor redundancy is utilized to diagnose the local and global confidence level of sensor data in real time,eliminate the fault data,and ensure the accuracy and reliability of data *** show that the network achieves state-of-the-art results in speed and accuracy,and can accurately detect the location of the target when some sensors are out of focus or out of *** fusion framework proposed in this paper is proved to be effective for intelligent vehicles in terms of real-time performance and reliability.

关键词： Autonomous vehicles Fault diagnosis and tolerance Object detection Data fusion

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The state-of-the-art synthetic strategies for SAPO-34 zeolite catalysts in methanol-to-olefin conversion

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National Science Review 2018年第4期5卷 542-558页

作者： qiming sun Zaiku Xie Jihong Yu State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University International Center of Future Science Jilin University SINOPEC Corporation Science and Technology Development Department

Methanol-to-olefin(MTO)conversion has proven to be one of the most successful non-petrochemical routes for producing light ***(SAPO)zeolite SAPO-34 is one of the best industrial catalysts for MTO conversion,but suffers from rapid deactivation due to the inherent diffusion bottleneck limited by the narrow eight-ring pore *** improve the MTO performance,considerable synthetic efforts have been devoted to decrease the crystal size of zeolites or introduce secondary larger pores in zeolite crystals to form hierarchical *** review mainly focuses on presenting the state-of-the-art synthetic strategies for nanosized and hierarchical SAPO-34 catalysts with excellent MTO ***,the industrialization of SAPO-34 catalysts for the MTO reaction,and some current problems and future prospects for the synthesis of SAPO-34 catalysts,are also pointed *** expect that this review can not only shed some light on the preparation of SAPO-34 catalysts,but also stimulate the future development of high-performance SAPO-34 catalysts to meet the increasing demands of the chemical industry.

关键词： methanol-to-olefin zeolites SAPO-34 hierarchically porous structure nanocrystals heterogeneous catalysis

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ORP8 acts as a lipophagy receptor to mediate lipid droplet turnover

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Protein & Cell 2023年第9期14卷 653-667页

作者： Maomao Pu Wenhui Zheng Hongtao Zhang Wei Wan Chao Peng Xuebo Chen Xinchang Liu Zizhen Xu Tianhua Zhou qiming sun Dante Neculai Wei Liu Metabolic Medicine Center International Institutes of Medicinethe Fourth Affiliated HospitalZhejiang University School of MedicineYiwu 322000China Joint Institute of Genetics and Genomics Medicine between Zhejiang University and University of Toronto Hangzhou 310058China National Center for Protein Science Shanghai Institute of Biochemistry and Cell BiologyShanghai Institutes of Biological SciencesChinese Academy of SciencesShanghai200031China

Lipophagy,the selective engulfment of lipid droplets(LDs)by autophagosomes for lysosomal degradation,is critical to lipid and energy *** we show that the lipid transfer protein ORP8 is located on LDs and mediates the encapsulation of LDs by autophagosomal *** function of oRP8 is independent of its lipid transporter activity and is achieved through direct interaction with phagophore-anchored LC3/*** lipophagy induction,ORP8 has increased localization on LDs and is phosphorylated by AMPK,thereby enhancing its affinity for LC3/*** of ORP8 or interruption of ORP8-LC3/GABARAP interaction results in accumulation of LDs and increased intracellular *** of ORP8 alleviates LD and triglyceride deposition in the liver of ob/ob mice,and Osbpl8 mice exhibit liver lipid clearance *** results suggest that ORP8 is a lipophagy receptor that plays a key role in cellular lipid metabolism.

关键词： ORP8 lipophagy lipid autophagy

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煤矸石-建筑固废砖填充材料正交试验及性能研究

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材料导报 2024年第S1期38卷 327-332页

作者：吴海宽张航启吴启红舒志乐杨咏漪李晋生杨瑞李祉臻李佳鑫孙启明西华大学应急管理学院成都610039 成都大学建筑与土木学院成都610106

利用正交试验设计(4因素4水平)对煤矸石-建筑固废砖填充材料(以下称膏体填充材料)的流动性与强度进行了测试。研究了粉煤灰掺量、废砖骨料取代率、质量浓度、减水剂掺量对膏体填充材料的坍落度、扩展度和早、中、后期抗压强度以及劈裂... 详细信息

利用正交试验设计(4因素4水平)对煤矸石-建筑固废砖填充材料(以下称膏体填充材料)的流动性与强度进行了测试。研究了粉煤灰掺量、废砖骨料取代率、质量浓度、减水剂掺量对膏体填充材料的坍落度、扩展度和早、中、后期抗压强度以及劈裂抗拉性能的影响,确定膏体填充材料的最优配合比,并对试验结果进行系统性分析。结果表明:各个因素对膏体填充材料流动性的影响显著,可总结为流动性随粉煤灰掺量、废砖骨料取代率、质量浓度的增加而下降,随减水剂掺量的增加而上升;各个因素对膏体填充材料早期抗压强度无明显影响;废砖取代率与减水剂掺量对膏体填充材料中、后期强度有一定的影响,当废砖骨料替代率为50%~75%、减水剂掺量为0.6%时,膏体填充材料抗压强度更高;粉煤灰掺量17%、废砖骨料取代率75%、质量浓度81%、减水剂掺量0.6%为最优组合。对选定方案的填充材料进行了微观形貌测试,说明该组合下配制出来的煤矸石膏体填充材料能保证强度,综合性能最佳。

关键词：煤矸石建筑固废膏体填充正交试验微观形貌

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Effects of extracellular vesicle-derived noncoding RNAs on pre-metastatic niche and tumor progression

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Genes & Diseases 2024年第1期11卷 176-188页

作者： Zhuang Chen qiming Wang Jinbo Liu Wenkang Wang Weitang Yuan Yang Liu Zhenqiang sun Chengzeng Wang Department of Colorectal Surgery The First Affiliated Hospital of Zhengzhou UniversityZhengzhouHenan 450052China Academy of Medical Sciences of Zhengzhou University ZhengzhouHenan 450001China Department of Internal Medicine Affiliated Cancer Hospital of Zhengzhou UniversityHenan Cancer HospitalZhengzhouHenan 450008China Department of Breast Surgery The First Affliated Hospital of Zhengzhou UniversityZhengzhouHenan 450052China Department of Radiotherapy Affiliated Cancer Hospital of Zhengzhou UniversityHenan Cancer HospitalZhengzhouHenan 450008China The First Affiliated Hospital of Zhengzhou University ZhengzhouHenan 450052China

A pre-metastatic niche(PMN)is a protective microenvironment that facilitates the colonization of disseminating tumor cells in future metastatic *** vesicles(EVs)play a role in intercellular communication by delivering cargoes,such as noncoding RNAs(ncRNAs).The pivotal role of extracellular vesicle-derived noncoding RNAs(EV-ncRNAs)in the PMN has attracted increasing *** this review,we summarized the effects of EV-ncRNAs on the PMN in terms of immunosuppression,vascular permeability and angiogenesis,inflammation,metabolic reprogramming,and fibroblast *** particular,we provided a comprehensive overview of the effects of EV-ncRNAs on the PMN in different ***,we discussed the promising clinical applications of EV-ncRNAs,including their potential as diagnostic and prognostic markers and therapeutic targets.

关键词： Biomarker Extracellular vesicles Noncoding RNAs

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EAB分子筛的合成及在甲醇制烯烃反应中的应用

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高等学校化学学报 2023年第8期44卷 25-35页

作者：杨颖楠孙启明苏州大学材料与化学化工学部化学科学国际合作创新中心江苏省先进负碳技术重点实验室苏州215123

甲醇制烯烃(MTO)反应提供了一条非石油路线制备低碳烯烃的新途径,发展新颖的催化材料是实现MTO反应性能提升的关键.本文探究了具有八元环孔道结构的EAB分子筛的合成条件和热稳定性;利用X射线衍射分析、扫描电子显微镜、电感耦合等离子... 详细信息

甲醇制烯烃(MTO)反应提供了一条非石油路线制备低碳烯烃的新途径,发展新颖的催化材料是实现MTO反应性能提升的关键.本文探究了具有八元环孔道结构的EAB分子筛的合成条件和热稳定性;利用X射线衍射分析、扫描电子显微镜、电感耦合等离子发射光谱及氨气程序升温脱附实验等表征了所制备分子筛的拓扑结构、晶体形貌、骨架组成和酸性位点;并发现向EAB分子筛孔道中引入K+和Cs+离子可以在550℃煅烧条件下使分子筛晶体结构保持稳定.通过向合成体系中加入晶种可以有效抑制杂晶的生成并提升晶化速率,EAB分子筛完全晶化的时间可缩短至3 d.此外,将制备的EAB分子筛催化剂应用于MTO催化反应,乙烯、丙烯和丁烯的总选择性最高可达87.2%,丙烯和乙烯的选择性比最高可达2.4.研究结果为开发新型MTO催化剂并实现低碳烯烃的比例调控提供借鉴.

关键词： EAB分子筛热稳定性水热合成甲醇制烯烃低碳烯烃

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Correction to:Metformin activates chaperone-mediated autophagy and improves disease pathologies in an Alzheimer disease mouse model

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Protein & Cell 2022年第3期13卷 227-229页

作者： Xiaoyan Xu Yaqin sun Xufeng Cen Bing Shan Qingwei Zhao Tingxue Xie Zhe Wang Tingjun Hou Yu Xue Mengmeng Zhang Di Peng qiming sun Cong Yi Ayaz Najafov Hongguang Xia Department of Biochemistry&Research Center of Clinical Pharmacy of The First Affiliated Hospital Zhejiang University School of MedicineHangzhou 310058China Liangzhu Laboratory Zhejiang University Medical CenterHangzhou 311121China Department of Cell Biology Harvard Medical SchoolBostonMA 02115USA Interdisciplinary Research Center on Biology and Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 201203China College of Pharmaceutical Sciences Hangzhou Institute of innovative MedicineZhejiang UniversityHangzhou 310058China Key Laboratory of Molecular Biophysics of Ministry of Education Hubei Bioinformatics and Molecular Imaging Key LaboratoryCollege of Life Science and TechnologyHuazhong University of Science and TechnologyWuhan 430074China

CORRECTION TO:PROTEIN CELL HTTPS://***/10.1007/S13238-021-00858-3 In legend of figure 1,this sentence“(C)293THK cells were treated as in a”should be corrected as“(C)293THK cells were treated as in(A)”.In legend of figure 2,“E-64D(10μmol/L)”in description of panel(B)should be *** section“Metformin activates chaperone-mediated autophagy”of RESULTS,E-64D in sentence“Metformininduced degradation of HK2 and PKM2 was blocked by lysosomal inhibitors(E-64D,Bafilomycin A1 and Leupeptin+NH4Cl)”should be removed.

关键词： Metformin Alzheimer removed

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