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Confined Mn^(2+) enables effective aerobic oxidation catalysis

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Science China Chemistry 2024年第5期67卷 1545-1553页

作者： Desheng Yuan Sicong Ma Xiao Kong Chi Zhang Lin Chen Chengsheng Yang Lihua Wang Zhen liu Lin Ye Yongmei liu Rui Ma Zhi-Pan liu Yifeng Zhu Yong Cao Xinhe Bao Department of Chemical Physics University of Science and Technology of ChinaHefei 230026China Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsCollaborative Innovation Center of Chemistry for Energy MaterialsFudan UniversityShanghai 200438China Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Materials and Chemistry University of Shanghai for Science and TechnologyShanghai 200093China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Institute of Advanced Fluorine-Containing Materials Zhejiang Normal UniversityJinhua 321004China State Key Laboratory of Catalysis National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Effective and mild activation of O_(2) is essential but challenging for aerobic oxidation. In heterogeneous catalysis, high-valence manganese oxide(e.g., +4) is known to be active for the oxidation, whereas divalent MnO is ineffective due to its limited capacity to supply surface oxygen and its thermodynamically unstable structure when binding O_(2) in reaction conditions. Inspired by natural enzymes that rely on divalent Mn^(2+), we discovered that confining Mn^(2+) onto the Mn_(2)O_(3) surface through a dedicated calcination process creates highly active catalysts for the aerobic oxidation of 5-hydroxymethylfurfural, benzyl alcohol, and *** Mn_(2)O_(3)-confined Mn^(2+) is undercoordinated and efficiently mediates O_(2) activation, resulting in 2–3 orders of magnitude higher activity than Mn_(2)O_(3) alone. Through low-temperature infrared spectroscopy, we distinguished low-content Mn^(2+) sites at Mn_(2)O_(3) surface, which are difficult to be differentiated by X-ray photoelectron spectroscopy. The combination of in-situ energydispersive X-ray absorption spectroscopy and X-ray diffraction further provides insights into the formation of the newly identified active Mn^(2+) sites. By optimizing the calcination step, we were able to increase the catalytic activity threefold *** finding offers promising frontiers for exploring active oxidation catalysts by utilizing the confinement of Mn^(2+)and oftenignored calcination skills.

关键词： confinement catalysis manganese oxide aerobic oxidation divalent Mn^(2+) operando spectroscopies

Comparative proteomics reveals the response and adaptation mechanisms of white Hypsizygus marmoreus against the biological stress caused by Penicillium

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Food Science and Human Wellness 2024年第3期13卷 1645-1661页

作者： Xiuqing Yang Sizhu Li Xiaohang Li Chenxiao Zhang Meijie liu Lizhong Guo Lin liu Hao Yu Shandong Provincial Key Laboratory of Applied Mycology School of Life SciencesQingdao Agricultural UniversityQingdao 266109China

White Hypsizygus marmoreus is a popular edible *** mycelium is easy to be contaminated by Penicillium,which leads to a decrease in its quality and *** could compete for limited space and nutrients through rapid growth and produce a variety of harmful gases,such as benzene,aldehydes,phenols,etc.,to inhibit the growth of *** mycelium.A series of changes occurred in *** proteome after contamination when detected by the label-free tandem mass spectrometry(MS/MS)*** proteins with up-regulated expression worked together to participate in some processes,such as the non-toxic transformation of harmful gases,glutathione metabolism,histone modification,nucleotide excision repair,clearing misfolded proteins,and synthesizing glutamine,which were mainly used in response to biological *** proteins with down-regulated expression are mainly related to the processes of ribosome function,protein processing,spliceosome,carbon metabolism,glycolysis,and *** reduction in the function of these proteins affected the production of the cell components,which might be an adjustment to adapt to growth *** study further enhanced the understanding of the biological stress response and the growth restriction adaptation mechanisms in edible *** also provided a theoretical basis for protein function exploration and edible mushroom food safety research.

关键词： Hypsizygus marmoreus Penicillium Proteomics Biological stress response Adaptation

A novel long persistent luminescent material CaGeO_(3):Tb^(3+)with photo-stimulation properties

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Journal of Rare Earths 2024年第7期42卷 1233-1239,I0002页

作者： Wei Meng Xiaoyan Fu Tongyan Lin Zewen liu Naihui Chen Jiaxu Zhang Runyao liu Rujun Yang Long Chen Hongwu Zhang School of Chemistry and Material Sciences Ludong UniversityYantai264025China College of Materials Science and Engineering Xiamen University of TechnologyXiamen361024China College of Materials Xiamen UniversityXiamen361005China

A novel green long afterglow material CaGeO_(3):Tb^(3+)was synthesized by high temperature solid phase *** to the experimental results,CaGeO_(3):Tb^(3+)is a green long persistent luminescent(LPL)material with excellent ***_(3):Tb^(3+)shows LPL emission peak at 442,490.9,548.7,588.5 and 623.8 nm,corresponding to ^(5)D_(3) to^(7)F_(4)and^(5)D_(4)to^(7)F_(J)(J=6,5,4,3)transitions of Tb^(3+).Its CIE coordinates are(0.27,0.50),indicating that the afterglow emission is close to the light of green *** addition,after the excitation source is turned off,the afterglow time is longer than 90 *** an interval of 7 h,the photo-stimulation luminescence(PSL)can be observed by using 980 nm laser cyclic *** thermoluminescence(ThL)results show that there are three types of traps in the material and their depths are 0.666,0.774 and 0.892 eV respectively,which are caused by the doping of Tb^(3+).All the results show that CaGeO_(3):Tb^(3+)is an excellent long afterglow luminescent material.

关键词： Long persistent luminescence Photo-stimulation Trap CaGeO_(3):Tb^(3+) Rare earths

Adhesion property of AlCrNbSiTi high-entropy alloy coating on zirconium:experimental and theoretical studies

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Nuclear Science and Techniques 2024年第8期35卷 79-91页

作者： Bao‑Liang Zhang Wen‑Guan liu Meng‑He Tu Can Fang Yan liu Yu‑Hui Wang Yong Hu Hui Wang China Institute of Atomic Energy Beijing 102413China Sino‑French Institute of Nuclear Engineering and Technology Sun Yat-Sen UniversityZhuhai 519082China School of Power and Mechanical Engineering Wuhan UniversityWuhan 430072China

Experimental scratch tests and first-principles calculations were used to investigate the adhesion property of AlCrNbSiTi high-entropy alloy(HEA)coatings on zirconium *** HEA and Cr coatings were deposited on zr alloy substrates using multi-arc ion plating technology,and scratch tests were subsequently conducted to estimate the adhesion property of the *** results indicated that Cr coatings had better adhesion strength than HEA coatings,and the HEA coatings showed *** special quasi-random structure approach was used to build HEA models,and Cr/zr and HEA/zr interface models were employed to investigate the cohesion between the coatings and zr substrate using first-principles *** calculated interface energies showed that the cohesion between the Cr coating and the zr substrate was stronger than that of the HEA coating with *** contrary to Al or Si in the HEA coating,Cr,Nb,and Ti atoms binded strongly with zr *** on the calculated elastic constants,it was found that low Cr and high Al content decreased the mechanical performances of HEA ***,this study demonstrated the utilization of a combined approach involving first-principles calculations and experimental studies for future HEA coating development.

关键词： High-entropy alloy coating Cr coating Adhesion property Scratch test First-principles calculation

Recent advances in vacancy engineering for reliable lithiumsulfur batteries

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Rare Metals 2024年第2期43卷 455-477页

作者： Wen-Dong liu Xiao Tang Jun-An Feng Chao-Yue Zhang Hao liu Chuan Shi Xiao-Xian Zhao Jian-Jun Song College of Physics School of Chemistry and Chemical EngineeringQingdao UniversityQingdao266071China Faculty of Science Centre for Clean Energy TechnologySchool of Mathematical and Physical SciencesUniversity of Technology SydneySydneyNSW2007Australia Department of Chemistry College of ScienceHebei Agricultural UniversityBaoding071001China

The high-energy-density and low-cost features endow lithium-sulfur batteries with broad application ***,many drawbacks,especially the detrimental shuttle effect,have hindered the further development of *** response,a lot of new structures have been applied to suppress the shuttle effect and promote the development of ***,vacancy engineering has gained the attention of researchers due to its unique electronic *** review aims to analyze the application of vacancy engineering in ***,the electrochemistry of LSBs has been systematically discussed and the existing challenges as well as improvement tactics of LSBs have also been ***,the preparation methods and characterization technologies of various vacancies are summarized,including oxygen vacancies,sulfur vacancies,selenium vacancies,other anion vacancies,cation vacancies,*** latest applications of vacancy engineering in LSBs are also summarized in this ***,some prospects and insights for further investigation and practical application of vacancy engineering in LSBs are put forward.

关键词： Lithium-sulfur batteries(LSBs) Defects Vacancy engineering Electronic structure Shuttle effect

Tuning electronic structure of RuO_(2)by single atom Zn and oxygen vacancies to boost oxygen evolution reaction in acidic medium

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Journal of Energy Chemistry 2024年第1期88卷 94-102,I0003页

作者： Qing Qin Tiantian Wang Zijian Li Guolin Zhang Haeseong Jang Liqiang Hou Yu Wang Min Gyu Kim Shangguo liu Xien liu College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Department of Chemistry City University of Hong KongHong Kong 999077China Department of Advanced Materials Engineering Chung-Ang UniversityAnseong-siGyeonggi-do 17546SeoulRepublic of Korea Beamline Research Division Pohang Accelerator Laboratory(PAL)Pohang 37673Gyeongsangbuk-doRepublic of Korea

The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane *** dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but ***,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from ***,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction *** a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.

关键词： Electrocatalyst Acidic oxygen evolution reaction Electronic structure engineering Durability Reaction barrier

High-performance Si/VO_(2)-nanorod heterojunction photodetector based on photothermoelectric effect for detecting human radiation

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Rare Metals 2024年第3期43卷 1177-1185页

作者： Fu-Hai Guo Lan-Zhong Hao Wei-Zhuo Yu Si-Qi Li Guan-Chu liu Jing-Yi Hao Yun-Jie liu College of Science China University of PetroleumQingdao266580China School of Materials Science and Engineering China University of PetroleumQingdao266580China

As a typical candidate of optoelectronic materials,vanadium dioxide(VO_(2))has wide applications in photodetectors(PDs),but is still challenging in largely enhancing the photodetecting performance for low-power human ***,high-performance Si/VO_(2)nanorods(NRs)heterojunction PDs based on the photothermoelectric(PTE)effect are *** uniform VO_(2)-NRs array films were deposited on Si by using magnetron sputtering technique,and a Si/VO_(2)heterojunctions were *** device exhibits a four-stage photoresponse and broadband photoresponse from ultraviolet to long-wavelength *** from the unique nanorods structure and the strong PTE effect,the fabricated device exhibits a large enhancement of the photodetecting performance,showing an ultrahigh photodetectivity of 1.6×10^(13)Jones and ultrafast response rates with a risingedge time of~65.0μs,three orders of magnitude higher than other VO_(2)-based ***,the device exhibits unique abilities to detect human radiation even when the human fingers are far away from the device surface up to 10.0 ***,the fabricated Si/VO_(2)devices can also be applied as breath sensors to distinguish different breathing *** results supply an effective route to design high-performance photodetectors toward detecting human thermal radiation and respiration.

关键词： Vanadium dioxide Heterojunction Photodetector Photothermoelectric Human radiation and respiration sensing

"Win-Win"Scenario of High Energy Density and Long Cycling Life in a Novel Na_(3.9)MnCr_(0.9)zr_(0.1)(PO_(4))_(3)Cathode

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Energy & Environmental Materials 2024年第1期7卷 83-90页

作者： Yao Wang Yukun liu Pingge He Junteng Jin Xudong Zhao Qiuyu Shen Jie Li Xuanhui Qu Yongchang liu Lifang Jiao Beijing Advanced Innovation Center for Materials Genome Engineering State Key Laboratory for Advanced Metals and MaterialsInstitute for Advanced Materials and TechnologyUniversity of Science and Technology BeijingBeijing 10083China Department of Chemistry and Biochemistry University of California1156 High StreetSanta CruzCA 95064USA Tianjin Key Laboratory for Photoelectric Materials and Devices School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

The development of high-energy and long-lifespan NASICON-type cathode materials for sodium-ion batteries has always been a research hotspot but a daunting *** Na_(4)MnCr(PO_(4))_(3)has emerged as one of the most promising high-energy-density cathode materials owing to its three-electron reactions,it still suffers from serious structural distortion upon repetitive charge/discharge processes caused by the Jahn-Teller active Mn^(3+).Herein,the selective substitution of Cr by zr in Na_(4)MnCr(PO_(4))_(3)was explored to enhance the structural stability,due to the pinning effect of zr ions and the≈2.9-electron reactions,as-prepared Na_(3.9)MnCr_(0.9)zr_(0.1)(PO_(4))_(3)/C delivers a high capacity retention of 85.94%over 500 cycles at 5 C and an ultrahigh capacity of 156.4 mAh g^(-1)at 0.1 C,enabling the stable energy output as high as 555.2 Wh kg^(-1).Moreover,during the whole charge/discharge process,a small volume change of only 6.7%was verified by in situ X-ray diffraction,and the reversible reactions of Cr^(3+)/Cr^(4+),Mn^(3+)/Mn^(4+),and Mn^(2+)/Mn^(3+)redox couples were identified via ex situ X-ray photoelectron spectroscopy *** intermittent titration technique tests and density functional theory calculations further demonstrated the fast reaction kinetics of the Na_(3.9)MnCr_(0.9)zr_(0.1)(PO_(4))_(3)/C *** work offers new opportunities for designing high-energy and high-stability NASICON cathodes by ion doping.

关键词： high energy density mechanism investigation NASICON-type cathodes sodium-ion batteries structure modification

Morphology effect on catalytic performance of ebullated-bed residue hydrotreating over Ni-Mo/Al_(2)O_(3)catalyst:a kinetic modeling study

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Green Chemical Engineering 2024年第1期5卷 60-67页

作者： Zhe liu Juncong Yuan Zongzhuang Sun Xiang Feng Yibin liu Huihong Zhu Chong Peng Chaohe Yang State Key Laboratory of Heavy Oil Processing China University of PetroleumQingdao266580China Dalian Research Institute of Petroleum and Petrochemicals SINOPECDalian116045China State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalian116024China

Upgrading of vacuum residue is of prime industrial significance due to the increasing demand for light *** the effect of catalyst morphology on vacuum residue hydrotreating performance by kinetic modeling is therefore of great ***,kinetic analysis of hydrodemetallization(HDM)and hydrodeconradsoncarbon-residue(HDCCR)performances on industrial Ni-Mo/Al_(2)O_(3)catalysts with spherical and cylindrical morphologies in ebullated-bed were evaluated for more than 1600 *** was found that the percentage of light impurities easier to be removed on spherical catalysts were 78.20%and 39.43%in HDM and HDCCR reactions,respectively,higher than 65.20%and 17.50%on cylindrical *** suggests that catalyst morphology affects the impurity removal ability and the impurity properties,resulting in better hydrotreating performance of spherical *** work not only combines catalyst morphology with impurity removal capability through kinetic modeling,but also provides new insights into the design of efficient hydrotreating catalysts.

关键词： Morphology effect Kinetic analysis Vacuum residue Hydrotreating