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Highly efficient hydrogen production from methanol by single nickel atoms anchored on defective boron nitride nanosheet

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Nano Research 2023年第7期16卷 8800-8808页

作者： Shengshu Yang Fang Zhang Haifa Qiu Ming Yang Fengjuan Qin Hao Tang Wenxing Chen Zhengang Liu Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 101408China Analytical and Testing Center Beijing Institute of TechnologyBeijing 100081China Department of Applied Physics the Hong Kong Polytechnic UniversityHong Kong 999077China Energy&Catalysis Center School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China

Exploiting inexpensive and effective nickel-based catalysts that produce hydrogen from liquid organic hydrogen carriers(LOHCs)is crucial to alleviating the global energy and environmental crisis.In this study,we report a rational strategy that can realize atomically dispersed Ni atoms anchored on vacancy-abundant boron nitride nanosheets(Ni1/h-BNNS)with high specific surface area(up to 622 m^(2)·g^(-1))and abundant hydroxyl groups for high efficient hydrogen production.Methanol dehydrogenation results show an excellent hydrogen production performance catalyzed by this Ni1/h-BNNS,as evidenced by a remarkably high H_(2) yield rate(1684.23 mol·mol_(Ni)^(-1)·h^(-1)),nearly 100%selectivity toward hydrogen and CO,and high anti-coking performance.Density functional theory(DFT)calculations reveal that the outstanding catalytic performance of Ni1/h-BNNS primarily originates from the unique coordinated environment of atomically dispersed Ni(Ni-B_(2)O_(2))and the synergistic interaction between Ni single atoms and the h-BNNS support.Specifically,the coordinated O atoms play a decisive role in promoting the activity of Ni,and the neighboring B sites significantly decrease the energy barriers for the adsorption of key intermediates of methanol dehydrogenation.This study offers a novel strategy for developing high-performance and stable single-atom Ni catalysts by precisely controlling single-atom sites on h-BN support for sustainable hydrogen production.

关键词： single-atom catalyst coordination environment boron nitride hydrogen production liquid organic hydrogen carriers

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Superoxide-like Cu/GO single-atom catalysts nanozyme with high specificity and activity for removing superoxide free radicals

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Nano Research 2022年第10期15卷 8804-8809页

作者： Mingju Lu Jialu Wang Guoyuan Ren Fengjuan Qin Zhiqiang Zhao Kai Li Wenxing Chen Yuqing Lin Department of Chemistry Capital Normal UniversityBeijing 100048China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

Although nanozyme has become an emerging area of research attracting extensive attention recently,the activity and specificity of currently reported nanozymes are generally lower than those of natural enzymes.Developing highly active and specific nanozymes is therefore extremely necessary and also remains a great challenge.Superoxide dismutase(SOD)catalyzes the disproportionation of cytotoxic O_(2)·^(−)into hydrogen peroxide and oxygen,and plays an important role in reducing human oxidative stress.In this work,we prepare Cu single-atom catalysts(Cu/GO SACs,GO=graphene oxide)through a simple and low-cost strategy at room temperature using Cu foam and graphene oxide.Cu/GO SACs can maintain excellent catalytic activity under harsh environment.Compared with the natural enzyme,SOD-like Cu/GO SAC nanozyme has higher catalytic activity and meanwhile,it does not possess the common properties of other mimic enzymes often existing in nanomaterials.Based on the excellent SOD-like enzyme activity of Cu/GO SACs,it successfully eliminates the active oxygen in cigarette smoke.This work not only provides a new idea for the design and synthesis of nanozymes with excellent SOD mimetic properties,but also is promising in the treatment of lung injury and inflammatory diseases related to free radical production.

关键词： Cu/graphene oxide(GO)single-atom catalysts(SACs) superoxide dismutase(SOD)-like activity activity specificity superoxide free radicals

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In situ decorating the surface and interlayer of montmorillonite with Co_(0.5)Ni_(0.5)Fe_(2)O_(4) nanoparticles: A sustainable, biocompatible colorimetric platform for H_(2)O_(2) and acetylcholine

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Nano Research 2022年第10期15卷 9319-9326页

作者： Xixi Zhu Hongyu Li Tao Wu Hui Zhao Kaili Wu Wenjing Xu Fengjuan Qin Wenxing Chen Jinlong Zheng qingyun Liu College of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266590China Beijing Advanced Innovation Center for Materials Genome Engineering Shunde Graduate SchoolSchool of Mathematics and PhysicsUniversity of Science and Technology BeijingBeijing 100083China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

Originated from nature and used for nature is a way of sustainable development.In this work,montmorillonite(MMT),a natural two-dimensional(2D)layered mineral,the surface and interlayer of which were nano-decorated by chemical synthesis technique was applied in biological detection field.Magnetic ferrite(Co_(0.5)Ni_(0.5)Fe_(2)O_(4))was anchored on the surface and intercalated in the interlayer of montmorillonite,which served as a competitive candidate of enzyme mimics.Cytotoxicity test toward HUVEC and Hela cells verified the good biocompatibility of Co_(0.5)Ni_(0.5)Fe_(2)O_(4)-MMT,guaranteeing its safety in biological applications.Based on the peroxidase-like activity of Co_(0.5)Ni_(0.5)Fe_(2)O_(4)-MMT,a colorimetric sensing platform for H_(2)O_(2) was established by a facile mix-anddetect approach with the detection limit of 0.565μM(3σ/slope).It was implied that the peroxidase-like activity of Co_(0.5)Ni_(0.5)Fe_(2)O_(4)-MMT was originated from generation of·OH and·O_(2)–produced from catalytic decomposition process of H_(2)O_(2).Coupled with cascaded catalytic reactions of ACh,a facile and efficient sensing platform for ACh with satisfactory anti-interference ability was established.Thus,all these remarkable features highlighted the superiority of Co_(0.5)Ni_(0.5)Fe_(2)O_(4)-MMT,and endowed it with a powerful competitiveness in the fields of environmental assessing,biosensing,and disease monitoring.

关键词： montmorillonite colorimetric assays hydrogen peroxide peroxidase-like activity nanozymes

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Interface electronic engineering of molybdenum sulfide/MXene hybrids for highly efficient biomimetic sensors

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Nano Research 2023年第1期16卷 1158-1164页

作者： Pengfei Wu Tingting You qingyuan Ren Hongyan Xi qingqing Liu Fengjuan Qin Hongfei Gu Yu Wang Wensheng Yan Yukun Gao Wenxing Chen Penggang Yin Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education School of ChemistryBeihang UniversityBeijing 100191China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Shanghai Synchrotron Radiation Facility Zhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China

Interface regulation plays a key role in the electrochemical performance for biosensors.By controlling the interfacial interaction,the electronic structure of active species can be adjusted effectively at micro and nano-level,which results in the optimal reaction energy barrier.Herein,we propose an interface electronic engineering scheme to design a strongly coupled 1T phase molybdenum sulfide(1T-MoS2)/MXene hybrids for constructing an efficient electrocatalytic biomimetic sensor.The local electronic and atomic structures of the 1T-MoS2/Ti3C2TX are comprehensively studied by synchrotron radiation-based X-ray photoelectron spectroscopy(XPS),as well as X-ray absorption spectroscopy(XAS)at atomic level.Experiments and theoretical calculations show that there are interfacial stresses,atomic defects and adjustable bond-length between MoS2/MXene nanosheets,which can significantly promote biomolecular adsorption and rapid electron transfer to achieve excellent electrochemical activity and reaction kinetics.The 1T-MoS2/Ti3C2TX modified electrode shows ultra high sensitivity of 1.198μA/μM for dopamine detection with low limit of 0.05μM.We anticipate that the interface electronic engineering investigation could provide a basic idea for guiding the exploration of advanced biosensors with high sensitivity and low detection limit.

关键词： MXene molybdenum sulfide interface electronic effect biomimetic sensor X-ray absorption spectroscopy

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Microbial degradation and its influence on components of coalbed gases in Enhong syncline, China

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International Journal of Mining Science and Technology 2013年第2期23卷 295-301页

作者： Lan fengjuan qin Yong Li Ming Tang Yonghong Guo Chen Zhang Fei School of Resource and Earth Science China University of Mining & Technology Key Laboratory of Coalbed Methane Resources and Reservoiring Process China Ministry of Education Yunnan Bureau of Coal Geological Survey

Coalbed gases (CBG) in Enhong syncline are characterized by high concentration of C2+ (C2-5 ), with the highest content of ethane over 30%. However, the concentrations of C2+ are not evenly distributed in the syncline. Based on the analysis of δ13C1 , δ13C2 , δ13C3 , δ13CO2 , δDCH4 of CBG and their origin diagrams in the normal and abnormal areas, this research shows that gases in both areas are thermogenic gases and the reason for the uneven distribution of C2+ is that the microbial degradation action on gases is stronger in the normal area than in the abnormal area. The secondary biologic gases in the normal area are mainly characterized by that the carbon isotopes become obviously lighter in methane and become heavier in ethane, whereas the molecular and isotopic compositions of CO2 change little. These features indicate that the secondary biologic gases are mainly generated by the microbial degradation of C2+ , not generated by the reduction of CO2 . The degradation process is selective to make the residual ethane being enriched in 13C and the generated methane rich in 12C.

关键词： Biologic gases C2+ Microbial degradation Stable isotopes Coalbed gases origin Enhong syncline

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Construction of Synergistic Co and Cu Diatomic Sites for Enhanced Higher Alcohol Synthesis

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CCS Chemistry 2023年第4期5卷 851-864页

作者： Gaofeng Chen Olga A.Syzgantseva Maria A.Syzgantseva Shuliang Yang Guihua Yan Li Peng Changyan Cao Wenxing Chen Zhiwei Wang Fengjuan Qin Tingzhou Lei Xianhai Zeng Lu Lin Weiguo Song Buxing Han College of Energy Xiamen UniversityXiamen 361102 Department of Chemistry Lomonosov Moscow State UniversityMoscow 119991 Fujian Engineering and Research Center of Clean and High-Valued Technologies for Biomass Xiamen Key Laboratory of Clean and High-Valued Utilization for BiomassXiamen 361102 College of Chemistry and Chemical Engineering Xiamen UniversityXiamen 361005 Beijing National Laboratory for Molecular Science CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100049 Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081 School of Environmental Engineering Henan University of TechnologyZhengzhou 450001 Institute of Urban and Rural Mining Changzhou UniversityChangzhou 213164

Higher alcohol synthesis(HAS)from syngas could efficiently alleviate the dependence on the traditional fossil resources.However,it is still challenging to construct high-performance HAS catalysts with satisfying selectivity,space–time yield(STY),and stability.Herein,we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix(Co/Cu–N–C).The Co/Cu–N–C is efficient for HAS and is among the best catalysts reported.With a COconversion of 81.7%,C2+OHselectivity could reach 58.5%with an outstanding C2+OH STY of 851.8 mg/g·h.We found that the N4–Co1 and Cu1–N4 showed an excellent synergistic effect.The adsorption of CO occurred on the Co site,and the surrounding nitrogen sites served as a hydrogen reservoir for the CO reduction reactions to form CHxCo.Meanwhile,the Cu sites stabilized a CHOCu species to interact with CHxCo,facilitating a barrier-free formation of C2 species,which is responsible for the high selectivity of higher alcohols.

关键词： dual atomic catalyst synergistic effect heterogeneous catalysis carbonmaterial higher alcohol synthesis

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Synthesis and Biological Activities of Novel s-Triazine Bridged Dinucleoside Analogs

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Chinese Journal of Chemistry 2011年第6期29卷 1205-1210页

作者： Shen, fengjuan Li, Xiaoliu Zhang, Xiaoyuan qin, Zhanbin Yin, qingmei Chen, Hua Zhang, Jinchao Key Laboratory of Chemical Biology of Hebei Province College of Chemistry and Environmental Science Hebei University Baoding Hebei 071002 China College of Science Hebei University of Science & Technology Shijiazhuang Hebei 050018 China

A series of novel dinucleosides linked by s-triazine were synthesized via the nucleophilic substitution reaction of amino nucleoside and cyanuric chloride in THF/H20. The biological activities of these novel dinucleos... 详细信息

关键词： dinucleoside s-triazine HIV-RT inhibition cyanuric chloride

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Electrocatalytic acidic oxygen evolution reaction:From nanocrystals to single atoms

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Aggregate 2021年第4期2卷 100-121页

作者： Nadia Ismail Fengjuan Qin Chaohe Fang Dan Liu Bihan Liu Xiangyu Liu Zi-long Wu Zhuo Chen Wenxing Chen Energy&Catalysis Center Department of Materials Physics and ChemistrySchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijingPeople’s Republic of China CNPC Research Institute of Petroleum Exploration&Development BeijingPeople’s Republic of China

Hydrogen is the most preferred choice as an energy source to replace the nonrenewable energy resources such as fossil fuels due to its beneficial features of abundance,ecofriendly,and outstanding gravimetric energy density.Splitting water through a proton exchange membrane(PEM)electrolyzer is a well-known method of hydrogen production.But the major impediment is the sluggish kinetics of oxygen evolution reaction(OER).Currently,scientists are struggling to build out an acid-stable electrocatalyst for OER with low overpotential and excellent stability.In this review,the reaction mechanism and characterization parameters of OER are introduced,and then the improvement method of metal nanocatalysts(noble metal catalysts and noble metal-free catalysts)in acidic media is discussed.Particularly,the application of single-atom catalysts in acidic OER is summarized,which is current researching focus.At the same time,we also briefly introduced the cluster phenomenon,which is easy to occur in the preparation of single-atom catalysts.More importantly,we summarized the in situ characterization methods such as in situ X-ray absorption spectroscopy,in situ X-ray photoelectron spectroscopy,and so forth,which are conducive to further understanding of OER reaction intermediates and active sites.Finally,we put forward some opinions on the development of acidic OER.

关键词： acidic media in situ characterization nanocatalysis oxygen evolution reaction single-atom catalysis

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The impact of the novel starch-lipid complexes on the glucolipids metabolism， inflammation， and gut dysbiosis of Type 2 diabetes mellitus rats

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Food Science and Human Wellness 2023年

作者： Yingshuang Lu Renbing qin Jin Wang fengjuan Xiang Yan Zhang Bowei Zhang Dancai Fan Huan Lv Xuemeng Ji Shujun Wang Shuo Wang State Key Laboratory of Food Nutrition and Safety Tianjin University of Science & Technology School of Food Science Henan Institute of Science and Technology Tianjin Key Laboratory of Food Science and Health School of Medicine Nankai University

It has been widely accepted that resistant starch (RS) provides numerous health benefits for human. In this research， we aimed at evaluating the performance of novel starch-lipid complexes， RS5， in comparison with RS2 on physical features， glucolipids metabolism， inflammation， and gut microbiota profiles of Type 2 diabetes mellitus (T2DM) rats. The T2DM model was established by streptozotocin injection to the high-fat-sugar fed rats. According to a serial of biochemical analyses， we found that RS5 diets were strongly correlated with enhanced homeostatic model assessment for insulin secretion (HOMA-IS)， high-density lipoprotein cholesterol (HDL-C)， adiponectin (ADP)， insulin action index (IAI)， glucagon-like peptide-1 (GLP1)， and short-chain fatty acids (SCFAs) in T2DM rats whilst negatively associated with the low-density lipoprotein (LDL-C) and inflammatory cytokines， showing the capabilities to ameliorate T2DM symptoms by regulation of glucolipid metabolism， gut metabolites， and inflammation. On the other hand， RS2-enriched supplementations were influential in the mediation of insulin secretion to improve glucose metabolism. The increasing evidence collected herein suggested that intestinal microbiota could mediate glucolipids metabolism and alleviate inflammation after certain microflora nourished by RS. In addition， RS intake made an impact on PI3K/AKT signaling pathway that might contribute to the improvement of glucose metabolism， insulin resistance， and inflammatory responses.

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激光测宽仪的调整、故障分析及快速处理方法

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河南冶金 2019年第3期27卷 47-50页

作者：覃凤娟安阳钢铁股份有限公司

介绍了安钢二轧2800轧线激光测宽仪的调整,对其常见故障进行了原因分析,并归纳总结出快速处理故障的方法和平时在调整和维护过程中特别需要注意的事项,让测宽仪维护变得更加方便、快捷,大大降低了激光测宽仪的故障率,也为厂里节约了成本。

关键词：激光测宽仪调整故障快速处理注意事项节约

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