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Controllable oxygen vacancies and morphology engineering:Ultra-high HER/OER activity under base–acid conditions and outstanding antibacterial properties

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Journal of Energy Chemistry 2022年第8期31卷 639-651,I0017页

作者： Hongyao Xue Alan Meng Tongqing Yang Zhenjiang Li Chunjun Chen College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266061ShandongChina Key Laboratory of Optic-electric Sensing and Analytical Chemistry for life Science MOECollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266061ShandongChina Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of Sciences 2Beijing 100190China School of Chemistry and Chemical Engineering University of Chinese Academy of SciencesBejing 100049China

Introducing vacancy defects and unique morphology is an effective strategy to improve the catalytic performance of transition metal compounds.However,precisely controlling the amount of vacancy defects remains challenging.Here,we propose a facile and efficient hydrothermal accompanying an annealing method to synthesize a series of Mn-doped CoO nanomaterials with controllable oxygen vacancies and unique morphology.The oxygen vacancies amount can be precisely controlled by adjusting the Mndoping content and is positively correlated with catalytic performance.It was found that the oxygen vacancies amount can reach up to 38.2%over the Mn-doped CoO nanomaterials,resulting in ultra-high hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalytic activity(HER:25.6 and 37 m V at 10 m A cm^(-2);OER:301 and 322 m V at 50 m A cm^(-2))under both basic and acidic conditions,while reaching 10 m A cm^(-2) for an ultra-low cell voltage of only 1.52 V,which exceeds that of Pt/C/RuO_(2) and all reported non-noble metal oxide catalysts.The DFT calculations reveal oxygen vacancies can optimize H*and HOO*intermediates adsorption free energy,thus improving the HER and OER performance.Interestingly,the Mn-doped CoO with rich oxygen vacancies exhibits excellent antibacterial properties in vitro of biomedicine.This work provides new ideas and methods for the rational design and precise control of vacancy defects in transition metal compounds and explores their potential application value in electrochemical water splitting and biomedical fields.

关键词： Oxygen vacancies Mn-doping HER OER Antibacterial

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Pt-surface oxygen vacancies coupling accelerated photo-charge extraction and activated hydrogen evolution

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Nano Research 2023年第4期16卷 4736-4741页

作者： Fangxu Dai Mingming Zhang Mingzhong Mi Zhenjiang Li Jun Xing Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyShandong Engineering Research Center for Marine Environment Corrosion and Safety ProtectionQingdao 266042China

Semiconductors-based heterogeneous photocatalytic water splitting has been extensively studied,but it still remains challenging to accelerate the separation of electron-hole pairs and facilitate the reaction kinetics.Here we report a general strategy to fabricate highly efficient Pt/TiO_(2)photocatalyst by coupling the Pt co-catalysts and surface oxygen vacancies(VO)of TiO_(2).TiO_(2)was pre-modified with alkali or alkaline earth metals ion solutions,which produce a large number of surface hydroxyl on TiO_(2).Subsequently,the photodeposited Pt sub-nanoparticles substitute surface hydroxyl and induce surface VO on TiO_(2).The coupling of Pt and surface VO on TiO_(2)can accelerate the extraction of photo-charges through the interaction of Pt-VO-Ti bonds and reduce the hydrogen evolution barrier,thereby promoting the photocatalytic activity.The synthesized Pt-VO-TiO_(2)sample exhibits a photocatalytic hydrogen evolution activity as high as 1.5 L·g^(−1)·h^(−1),which is 2.2 times that of traditional Pt/TiO_(2).Our findings indepth understand the synergistic effect of co-catalysts and defects on photocatalysis and open up new possibilities for achieving robust photocatalytic water splitting.

关键词： oxygen vacancies co-catalyst surface hydroxyl photocatalytic hydrogen evolution reaction(HER)

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Selenium vacancies enable efficient immobilization and bidirectional conversion acceleration of lithium polysulfides for advanced li-S batteries

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Nano Research 2022年第8期15卷 7234-7246页

作者： Yuanchang li Zhenfang Zhou Yong li Zhonghua Zhang Xiaosong Guo Jing liu Changming Mao Zhenjiang Li Guicun li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China

Heterostructures composed of oxides and sulfides(nitrides or carbides)show great potential as sulfur host additives because of the strong adoptability of oxides and catalytic capability of sulfides towards the notorious lithium polysulfides(liPSs).However,the migration and conversion pathway of liPSs is seriously confined at a localized interface with inadequate active sites.In this work,the introduction of selenium vacancies into VSe_(2−x)has been demonstrated to successfully synergize the adsorbability and catalytic reactions of liPSs at an integrated functional surface.The N-doped carbon nanosheets-assembled flower architectures embedded with selenium vacancy-rich VSe_(2−x)and partial vanadium oxides have been controllably synthesized and employed as the cathode additives for lithium-sulfur(li-S)batteries.Both the experiments and first-principle calculations reveal their strong adsorption to liPSs and their bidirectional catalytic functionality towards the conversion between S8 and li_(2)S.As expected,the charge and discharge kinetics of VSe_(2−x)containing sulfur cathodes is fundamentally improved(an outstanding rate capabilitiy with 693.7 mAh·g^(−1)at 2 C,a remarkable long-term cyclability within 1,000 cycles at 2 C with S loading 2.27 mg·cm^(−2),and an excellent areal capacity with 3.44 mAh·cm^(−2)within 100 cycles at 0.5 C).This work presents an effective resolution to couple the adsorbability and catalytic reactions of liPSs at the material design perspective,and the insights on bidirectional catalytic functionality are of vital to develop functional materials for advanced li-S batteries.

关键词： lithium-sulfur batteries selenium vacancies vanadium selenide bidirectional catalysis conversion kinetics

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Inertial Motion Tracking on Mobile and Wearable Devices:Recent Advancements and Challenges

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Tsinghua Science and Technology 2021年第5期26卷 692-705页

作者： Zhipeng Song Zhichao Cao Zhenjiang Li Jiliang Wang Yunhao liu the School of Software Tsinghua UniversityBeijing 100084China the Department of Computer Science and Engineering Michigan State UniversityMichiganMI 48824USA the Department of Computer Science City University of Hong KongHong Kong 999077China the Department of Automation and the Global Innovation eXchange Institute(GIX) Tsinghua UniversityBeijing 100084China

Motion tracking via Inertial Measurement Units(IMUs)on mobile and wearable devices has attracted significant interest in recent years.High-accuracy IMU-tracking can be applied in various applications,such as indoor navigation,gesture recognition,text input,etc.Many efforts have been devoted to improving IMU-based motion tracking in the last two decades,from early calibration techniques on ships or airplanes,to recent arm motion models used on wearable smart devices.In this paper,we present a comprehensive survey on IMU-tracking techniques on mobile and wearable devices.We also reveal the key challenges in IMU-based motion tracking on mobile and wearable devices and possible directions to address these challenges.

关键词： Inertial Measurement Units(IMUs) motion tracking accelerometer gyroscope magnetometer sensor fusion

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Bifunctional core–shell co-catalyst for boosting photocatalytic CO_(2) reduction to CH_(4)

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Nano Research 2024年第3期17卷 1259-1266页

作者： Fangxu Dai Mingming Zhang Jishu Han Zhenjiang Li Shouhua Feng Jun Xing Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyShandong Engineering Research Center for Marine Environment Corrosion and Safety ProtectionQingdao 266042China

Solar-light-driven CO_(2) reduction CO to CH_(4) and C2H6 is a complex process involving multiple elementary reactions and energy barriers.Therefore,achieving high CH_(4) activity and selectivity remains a significant challenge.Here,we integrate bifunctional Cu2O and Cu-MOF(MOF=metal-organic framework)core–shell co-catalysts(Cu2O@Cu-MOF)with semiconductor TiO_(2).Experiments and theoretical calculations demonstrate that Cu2O(Cu+facilitates charge separation)and Cu-MOF(Cu2+improves the CO_(2) adsorption and activation)in the core–shell structure have a synergistic effect on photocatalytic CO_(2) reduction,reducing the formation barrier of the key intermediate*COOH and*CHO.The photocatalyst exhibits high CH_(4) yield(366.0μmol·g^(-1)·h^(-1)),efficient electron transfer(3283μmol·g^(-1)·h^(-1))and hydrocarbon selectivity(95.5%),which represents the highest activity of Cu-MOF-based catalysts in photocatalytic CO_(2) reduction reaction.This work provides a strategy for designing efficient photocatalysts from the perspective of precise regulation of components.

关键词： bifunctional co-catalyst core–shell photocatalytic CO_(2)reduction

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Surface reconstruction,doping and vacancy engineering to improve the overall water splitting of CoP nanoarrays

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Nano Research 2023年第1期16卷 228-238页

作者： Yongkai Sun Wenyuan Sun lihong Chen Alan Meng Guicun li Lei Wang Jianfeng Huang Aili Song Zhenhui Zhang Zhenjiang Li College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266061China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China Key Laboratory of Optic-electric Sensing and Analytical Chemistry for life Science MOE College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China School of Material Science and Engineering International S&T Cooperation Foundation of Shaanxi ProvinceXi’an Key Laboratory of Green Manufacture of Ceramic MaterialsShaanxi University of Science and TechnologyXi’an 710021China Qingdao Huanghai University Qingdao 266000China

Development of a general regulatory strategy for efficient overall water splitting remains a challenging task.Herein,a simple,costfairness,and general fluorination strategy is developed to realize surface reconstruction,heteroatom doping,and vacancies engineering over cobalt phosphide(CoP)for acquiring high-performance bifunctional electrocatalysts.Specifically,the surface of CoP nanoarrays(NAs)becomes rougher,meanwhile F doped into CoP lattice and creating amounts of P vacancies by fluorination,which caused the increase of active sites and regulation of charge distribution,resulting the excellent electrocatalyst performance of F-CoP NAs/copper foam(CF).The optimized F-CoP NAs/CF delivers a lower overpotential of only 35 mV at 10 mA·cm^(−2)for hydrogen evolution reaction(HER)and 231 mV at 50 mA·cm^(−2)for oxygen evolution reaction(OER),and the corresponding overall water splitting requires only 1.48 V cell voltage at 10 mA·cm^(−2),which are superior to the most state-of-theart reported electrocatalysts.This work provides an innovative and feasible strategy to construct efficient electrocatalysts.

关键词： fluorination surface reconstruction F atom doping P vacancies overall water splitting

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Intercalation-deintercalation design in MXenes for high-performance supercapacitors

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Nano Research 2022年第4期15卷 3213-3221页

作者： Zhenjiang Li Jun Dai Yiran li Changlong Sun Alan Meng Renfei Cheng Jian Zhao Minmin Hu Xiaohui Wang School of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266061China College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266061China Department of Mechanical Engineering City University of Hong KongHong Kong 999077China State Key Laboratory Base of Eco-chemical Engineering College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China

MXene is a new intercalation pseudocapacitive electrode material for supercapacitor application.Intensifying fast ion diffusion is significantly essential for MXene to achieve excellent electrochemical performance.The expansion of interlayer void by traditional spontaneous species intercalation always leads to a slight increase in capacitance due to the existence of species sacrificing the smooth diffusion of electrolyte ions.Herein,an effective intercalation-deintercalation interlayer design strategy is proposed to help MXene achieve higher capacitance.Electrochemical cation intercalation leads to the expansion of interlayer space.After electrochemical cation extraction,intercalated cations are deintercalated mostly,leaving a small number of cations trapped in the interlayer silt and serving as pillars to maintain the interlayer space,offering an open,unobstructed interlayer space for better ion migration and storage.Also,a preferred surface with more-O terminations for redox reaction is created due to the reaction between cations and-OH terminations.As a result,the processed MXene delivers a much improved capacitance compared to that of the original Ti_(3)C_(2)T_(x)electrode(T stands for the surface termination groups,such as-OH,-F,and-O).This study demonstrates an improvement of electrochemical performance of MXene electrodes by controlling the interlayer structure and surface chemistry.

关键词： MXene electrochemical ion intercalation−deintercalation interlayer design supercapacitor energy storage

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A case of acute renal injury and renal artery stenosis caused by cholesterol crystal embolization after coronary stenting:Improved by a combination therapy

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Chronic Diseases and Translational Medicine 2021年第3期7卷 206-210页

作者： Xiaohui Yan Yanting Zhu Xiaoming Wang Zhenjiang Li Center of Nephropathy and Hemodialysis Shaanxi Provincial People's HospitalXi'anShaanxi 710061China

Cholesterol crystal embolism(CCE),characterized by diverse clinical presentation,limited therapeutic options and poor long-term outcomes,is a multi-systemic disease in which cholesterol crystals emboli released from atherosclerotic plaques of the aorta or other major arteries occlude small arteries and subsequently lead to a foreign-body giant cell granuloma inflammatory reaction.1 Invasive vascular procedure.

关键词： cholesterol arteries clinical

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Porous needle-like Fe-Ni-P doped with Ru as efficient electrocatalyst for hydrogen generation powered by sustainable energies

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Nano Research 2023年第2期16卷 2428-2435页

作者： Yue Wang Zhi Chen Qichang li Xinping Wang Weiping Xiao Yunlei Fu Guangrui Xu Bin li Zhenjiang Li Zexing Wu Lei Wang Key Laboratory of Eco-chemical Engineering International Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Science Nanjing Forestry UniversityNanjing 210037China Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266061China

Electrocatalytic water electrolysis,involving hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),two halfreactions,is an eco-friendly approach toward hydrogen production.In this work,needle-like Ru-Fe-Ni-P on NiFe foam is prepared through corrosive engineering and following a low-temperature phosphorization procedure for overall water-splitting.The as-designed Ru-Fe-Ni-P exhibits a porous needle-like structure,surface,and binder-free merits,and then can expose rich active sites,favor the transportation of mass/electron,and accelerate the reaction kinetics during catalytic process.Then,the synthesized Ru-Fe-Ni-P owns remarkable catalytic performance for HER,with 18 and 67 mV to reach 10 mA·cm^(−2)in alkaline and neutral media.Moreover,a low cell voltage of 1.51 V is required to produce a current of 10 mA·cm^(−2)in a two electrode electrolyzer with excellent stability.Interestingly,sustainable energies can power the electrolyzer effectively with abundant hydrogen generation.

关键词： metal phosphide needle-like morphology hydrogen generation overall water splitting

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Insight into the synergistic effect of defect and strong interface coupling on ZnIn_(2)S_(4)/CoIn_(2)S_(4)heterostructure for boosting photocatalytic H_(2) evolution

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Journal of Energy Chemistry 2024年第5期92卷 151-161页

作者： Xuehua Wang Tianyu Shi Xianghu Wang Aili Song Guicun li Lei Wang Jianfeng Huang Alan Meng Zhenjiang Li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Key Laboratory of Optic-electric Sensing and Analytical Chemistry for life Science MOECollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina Qingdao Huanghai University Qingdao 266000ShandongChina School of Material Science and Engineering International S&T Cooperation Foundation of Shaanxi ProvinceXi’an Key Laboratory of Green Manufacture of Ceramic MaterialsShaanxi University of Science and TechnologyXi’an 710021ShaanxiChina

Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)S_(4)(HVs-ZIS)and CoIn_(2)S_(4)(CIS)via a defect-guided heteroepitaxial growth strategy.The strong interface coupling induces adequate carriers exchanging passageway between HVs-ZIS and CIS,enhancing the internal electric field(IEF)in the ZnIn_(2)S_(4)/CoIn_(2)S_(4)(HVs-ZIS/CIS)heterostructure.The defect structure in HVs-ZIS induces an additional defect level,improving the separation efficiency of photocarriers.Moreover,promoted by the IEF and intimate heterointerface,photogenerated electrons trapped by the defect level can migrate to the valence band of CIS,contributing to massive photogenerated electrons with intense reducibility in HVs-ZIS/CIS.Consequently,the HVs-ZIS/CIS heterostructure performs a boosted H_(2)evolution activity of 33.65 mmol g^(-1)h^(-1).This work highlights the synergistic effects of defect and strong interface coupling in regulating carrier transfer and paves a brave avenue for constructing efficient heterostructure photocatalysts.

关键词： Defect-guided heteroepitaxial growth Heterointerface coupling Photocatalytic H_(2)evolution Mechanism HVs-ZIS/CIS

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