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Cu/Mo2C synthesized through Anderson-type polyoxometalates modulate interfacial water structure to achieve hydrogen evolution at high current density

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Nano Research 2024年第4期17卷 2546-2554页

作者： Dunyuan Jin fen qiao Yan Zhou Junfeng Wang Kecheng Cao Jing Yang Jikang Zhao Lei Zhou Haitao Li School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013China School of Physical Science and Technology and Shanghai Key Laboratory of High-resolution Electron Microscopy ShanghaiTech UniversityShanghai 201210China Institute for Energy Research Jiangsu UniversityZhenjiang 212013China

The development of efficient non-precious metal catalysts is important for the large-scale application of alkaline hydrogen evolution reaction(HER).Here,we synthesized a composite catalyst of Cu and Mo_(2)C(Cu/Mo_(2)C)using Anderson-type polyoxometalates(POMs)synthesized by the facile soaking method as precursors.The electronic interaction between Cu and Mo_(2)C drives the positive charge of Cu,alleviating the strong adsorption of hydrogen at the Mo site by modulating the d-band center of Mo_(2)C.By studying the interfacial water structure using in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS),we determined that the positively charged Cu crystals have the function of activating water molecules and optimizing the interfacial water structure.The interfacial water of Cu/Mo_(2)C contains a large amount of free water,which could facilitate the transport of reaction intermediates.Due to activated water molecules and optimized interfacial water structure and hydrogen adsorption energy,the overpotential of Cu/Mo_(2)C is 24 mV at a current density of 10 mA·cm^(-2) and 178 mV at a current density of 1000 mA·cm^(-2).This work improves catalyst performance in terms of interfacial water structure optimization and deepens the understanding of water-mediated catalysis.

关键词： electrocatalytic hydrogen production interfacial water charge transport d band center in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)

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ZIF-8 modified by isocyanate as a photocatalytic antibacterial agent

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Rare Metals 2024年第6期43卷 2708-2718页

作者： Yi-Ning Zhang Zhen Pei Zi-Hao Wang Chong-En Wang fen-fen Liang Li-qiao Wei College of Architecture Taiyuan University of Technology Key Laboratory of Interface Science and Engineering in Advanced Materials of Taiyuan University of Technology Ministry of Education Department of Materials Science and Engineering Shanxi Institute of Technology Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering

Zeolite imidazole skeleton（ZIF-8） is a promising option for self-cleaning of building exterior walls due to its large specific surface area,high antibacterial activity and low biotoxicity.However,it suffers from low antibacterial efficiency and yield under visible light irradiation.To address the issues,we developed the photocatalytic materials T-ZIF-8-TDI（thermally treated-ZIF-8-toluene 2,4-diisocyanate） by modifying ZIF-8 with thermal oxygen sensitization and chemical bonding.The results show that the yield of T-ZIF-8-TDI photocatalytic antibacterial agent is increased to 11.5 times of that of T-ZIF-8,while maintaining the crystal structure of T-ZIF-8 and thermal stability up to 60℃.Furthermore,T-ZIF-8-TDI exhibits extended optical response range to the nearinfrared region,significantly narrowed band gap,improved photogenerated elec tron-hole separation efficiency,reduced recombination rate,and excellent photocatalytic performance.When the concentration of antibacterial agent is 600 mg·L-1,the antibacterial rate of Escherichia coli（E.coli） reaches 99.99% irradiated by visible light for30 min,and when the concentration of antibacterial agent is 200 mg·L-1,the antibacterial rate of Staphylococcus aureus（S.aureus） reaches 99.99% irradiated by visible light for 25 min.We also analyzed the reasons in detail from the aspects of bacterial species and antibacterial mechanism,and proposed the antibacterial mechanism of·O2-and h+as the main active species.These findings suggest that T-ZIF-8-TDI photocatalytic antibacterial agent has potential for use in self-cleaning of building exterior walls.

关键词： ZIF-8 Hot oxygen sensitization Modified by isocyanate Antimicrobial performance Photocatalytic antibacterial mechanism

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Photo-induced 1,2-aryl migration of 2-chloro-1-arylpropanone under batch and flow conditions:Rapid,scalable and sustainable approach to 2-arylpropionic acids

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Chinese Chemical Letters 2024年第2期35卷 366-369页

作者： qiao Li Minjie Liu Meifen Jiang Li Wan Yingtang Ning fen-Er Chen College of Chemical Engineering Zhejiang University of TechnologyHangzhou 310014China Engineering Center of Catalysis and Synthesis for Chiral Molecules Fudan UniversityShanghai 200433China Shanghai Engineering Center of Industrial Catalysis for Chiral Drugs Shanghai 200433China Institute of Pharmaceutical Science and Technology Zhejiang University of TechnologyHangzhou 310014China

We report the photo-mediated 1,2-aryl migration of 2‑chloro-1-arylpropanones to 2-arylpropionic acids using HCOONa as an acid scavenger.This pragmatically focused study obviates the multiple-step sequence in the industrially employed,ZnO-promoted rearrangement strategy,and offers rapid access to various 2-arylpropionic acids under environmentally friendly conditions.Furthermore,the successful transfer of this batch photochemistry to a continuous flow platform led to improved scalability and enabled the gram-scale synthesis of loxoprofen.

关键词： Green chemistry Flow chemistry 2-Arylpropionic acids Photo-Favorskii reaction

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Prevalence and risk factors of depression among patients with perianal fistulizing Crohn’s disease

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World Journal of Psychiatry 2024年第5期14卷 715-725页

作者： Jing Li Wing-Yi Ng Li-Chao qiao fen Yuan Xing Lan Li-Bei Zhu Bo-Lin Yang Zhong-Qiu Wang Department of Radiology Jiangsu Province Hospital of Chinese Medicine Affiliated Hospital of Nanjing University of Chinese MedicineNanjing 210029Jiangsu ProvinceChina Department of Acupuncture and Rehabilitation Jiangsu Province Hospital of Chinese Medicine Affiliated Hospital of Nanjing University of Chinese MedicineNanjing 210029Jiangsu ProvinceChina Department of Colorectal Surgery Jiangsu Province Hospital of Chinese Medicine Affiliated Hospital of Nanjing University of Chinese MedicineNanjing 210029Jiangsu ProvinceChina

BACKGROUND Psychological distress,especially depression,associated with perianal fistulizing Crohn’s disease(PFCD)is widespread and refractory.However,there is a surprising paucity of studies to date that have sought to identify the prevalence and risk factors of depression associated with PFCD.AIM To estimate the prevalence of depressive symptoms and investigate the depression-related risk factors in patients with PFCD.METHODS The study was conducted in the form of survey and clinical data collection via questionnaire and specialized medical staff.Depressive symptoms,life quality,and fatigue severity of patients with PFCD were assessed by Patient Health Questionnaire-9,Inflammatory Bowel Disease Patient Quality of Life Questionnaire(IBDQ),and Inflammatory Bowel Disease(IBD)Fatigue Patient Self-assessment Scale.The basic demographic information,overall disease features,perianal clinical information,and laboratory inflammation indicators were also gathered.Multivariate regression analysis was ultimately used to ascertain the risk factors of depression associated with PFCD.RESULTS A total of 123 patients with PFCD were involved,and 56.91%were suffering from depression.According to multivariate logistic regression analysis,Perianal Disease Activity Index(PDAI)score[odds ratio(OR)=0.69,95%confidence interval(CI):0.50 to 0.95],IBDQ score(OR=0.93,95%CI:0.88 to 0.97),modified Van Assche index(OR=1.24,95%CI:1.01 to 1.53),and IBD Fatigue score(OR=1.72,95%CI:1.23 to 2.42)were independent risk factors of depression-related prevalence among patients with PFCD(P<0.05).Multiple linear regression analysis revealed that the increasing perianal modified Van Assche index(βvalue=0.166,95%CI:0.02 to 0.31)and decreasing IBDQ score(βvalue=-0.116,95%CI:-0.14 to-0.09)were independently associated with the severity of depression(P<0.05).CONCLUSION Depressive symptoms in PFCD patients have significantly high prevalence.PDAI score,modified Van Assche index,quality of life,and fatigue severity were the main independent risk factors.

关键词： Crohn’s disease Fistula Depression Inflammatory bowel diseases Risk factors

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Strategies for enhancing conductivity of colloidal nanocrystals and their photoelectronic applications

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Journal of Energy Chemistry 2020年第9期29卷 29-42,I0002页

作者： fen qiao Yi Xie School of Energy&Power Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070HubeiChina

Semiconductor colloidal nanocrystals(NCs)have size-and shape-dependent optoelectronic properties due to the quantum confinement effect,and are considered to be promising optoelectronic materials.Among them,Ⅱ-Ⅵ(CdSe,CdS,CdTe,etc.)andⅣ-Ⅵ(PbSe,PbTe,PbS,etc.)have been widely studied as representative colloidal NCs.However,the surfactant used in its synthesis progress results in the NCs surface covered by an insulating shell,which greatly affects the exciton separation and carrier transport of colloidal NCs-based photovoltaic devices.Therefore,how to design high-efficiency optoelectronic devices by improving the transport performance of carriers has been a great challenge.The key issues in the research ofⅡ-Ⅵ(CdSe,CdS,CdTe,etc.)andⅣ-Ⅵ(PbSe,PbTe,PbS,etc.)colloidal NCs were summarized,including synthesis strategy,morphology/size adjustment,surface ligand design,improvement of conductivity and their optoelectronic properties.The influence of surface ligands on the stability and dispersion of NCs was firstly introduced,and then strategies of improving electrical conductivity of NCs were discussed,such as ligands exchange,doping,self-assembly and plasmons,which provided a good foundation for the subsequent preparation of optoelectronic devices.The future development direction of NCs optoelectronic devices is expounded from the aspects of materials composition,comprehensive preparation and flexible processing of colloidal NCs.

关键词： Colloidal nanocrystal Surface engineering Conductivity Photoelectronic device

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Embedding partial sulfurization of iron-cobalt oxide nanoparticles into carbon nanofibers as an efficient electrode for the advanced asymmetric supercapacitor

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Tungsten 2023年第1期5卷 118-129页

作者： Wen-Jie Liu Ming Yuan Jia-Biao Lian Guo-Chun Li Qiu-Ping Li fen qiao Yan Zhao Institute for Energy Research School of Energy and Power EngineeringJiangsu UniversityZhenjiang 212013China Fuzhou Medical College of Nanchang University Fuzhou 344000China College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021China

In this paper,a series of partially sulfurized iron-cobalt oxide(FCOS) nanoparticles were embedded in carbon nanofibers(FCOS@CNF) via a simple electrospinning method and followed by a hydrothermal sulfurization process.The sulfurization degree of iron-cobalt oxide nanoparticles can be further controlled by tuning the hydrothermal reaction time.The self-supported FCOS@CNF samples with hierarchical nanostructure can not only effectively prevent the detaching of the FCOS nanoparticles but also provide abundant electrochemical active sites.When used as a supercapacitor electrode,the FCOS@CNF^(-1)0 electrode presents a high specific capacitance(1039 F·g^(-1)at 1 A·g^(-1)),a good rate performance(over 69.4%of capacitance retention from 1 to 15 A·g^(-1)),and a long cycle lifespan(88.3% of capacitance retention after 4000 cycles at10 A·g^(-1)).A unique(FCOS@CNF^(-1)0//F-RGO) asymmetric supercapacitor device was assembled using the FCOS@CNF^(-1)0 sample as the positive electrode and the freeze-dried reductive graphene oxide(F-RGO) as the negative electrode.The hybrid device exhibits excellent electrochemical properties,including a high specific capacity,a long cycle life(86% after5000 cycles at 10 A·g^(-1)),and a maximum energy density of 24.2 Wh·kg^(-1)@725.4 W·kg^(-1).

关键词： Electrospinning Carbon nanofibers Transition metal sulfur oxide Supercapacitors

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Hierarchical polypyrrole@cobalt sulfide-based flexible on-chip microsupercapacitors with ultrahigh energy density for selfcharging system

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Nano Research 2023年第1期16卷 555-563页

作者： Yan Zhao Jihua Zheng Jing Yang Wenjie Liu fen qiao Jiabiao Lian Guochun Li Tao Wang Jiangwei Zhang Limin Wu College of Energy Material and Chemistry College of Chemistry and Chemical EngineeringInner Mongolia UniversityHohhot 010021China Institute for Energy Research School of Energy&Power EngineeringJiangsu UniversityZhenjiang 212013China Department of Materials Science Fudan UniversityShanghai 200433China Key Laboratory of Power Station Energy Transfer Conversion and System Ministry of EducationNorth China Electric Power UniversityBeijing 102206China

Herein,we prepare the unique hierarchical polypyrrole@cobalt sulfide(PPy-hs@CoS)hollow sphere-based nanofilms as interdigitated electrodes for flexible on-chip micro-supercapacitors(MSC).Benefiting from the excellent flexibility and high electrical conductivity of PPy-hs combined with the great electrochemical activity of CoS,such PPy-hs@CoS composite material can not only inhibit the volume expansion of PPy but also promote the diffusion of the electrolyte ions.The PPy-hs@CoS filmbased electrode delivers a greatly improved specific capacitance and small resistance.Density functional theory calculations infer that OH−prefers to bind to PPy on CoS@PPy and confirms the synergistic effect of each component for enhanced reaction kinetics.A quasi-solid-state on-chip flexible asymmetric MSC based on PPy-hs@CoS and activated carbon(AC)microelectrodes exhibits large areal-specific capacitance(131.9 mF/cm2 at 0.3 mA/cm2),ultrahigh energy density(0.041 mWh/cm2@0.224 mW/cm2 and 25.6 mWh/cm3@140.6 mW/cm3),and long cycle lifespan.We demonstrate the possibility to scale up the PPy-hs@CoS nanofilm microelectrode by arranging two of our asymmetric MSC in series and parallel connections,which respectively increase the output voltage and current.A self-charging system by connecting our asymmetric MSCs with a piece of commercial solar cells is developed as a potential possible mode for future highly durable and high-voltage integrated electronics.

关键词： polypyrrole cobalt sulfide adsorption energy on-chip micro-supercapacitor self-charging device

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Coral-like cobalt selenide/carbon nanosheet arrays attached on carbon nanofibers for high-rate sodium-ion storage

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Rare Metals 2023年第3期42卷 916-928页

作者： Jin-Zhi Hu Wen-Jie Liu Ji-Hua Zheng Guo-Chun Li Yong-feng Bu fen qiao Jia-Biao Lian Yan Zhao Institute for Energy Research School of Energy and Power EngineeringJiangsu UniversityZhenjiang 212013China College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021China

Cobalt selenide(CoSe_(2))has become a promising anode material for sodium-ion batteries(SIBs)due to its stable chemical properties,environmental friendliness,and high theoretical capacity.However,the undesirable rate capacity and cycle stability of the anode materials largely limit its applications for SIBs due to the relatively low electronic conductivity and huge volume change during the Na+insertion/extraction.In this study,electrostatic spinning combined with a wet chemical method is employed to synthesize coral-like composite material(CNF@c-CoSe_(2)/C),which is composed of CoSe_(2)/carbon nanosheet arrays(CoSe_(2)/C)and carbon nanofibers(CNFs).CoSe_(2)/C nanoflakes derived from metal-organic frameworks(MOFs)with high surface area and the porous structure can inhibit the pulverization and amorphization of CoSe_(2) during charge and discharge processes,thus significantly keeping the stability of the microstructure.CNF can limit the overgrowth of nanosheets and serve as a conductive skeleton.Compared to two-dimensional CoSe_(2)/C nanoflakes and pure CoSe_(2) nanoparticles,the composite can expose more active sites and effectively accelerate the diffusion of Na+,which displays enhanced rate capability(266.5 mAh·g^(-1) at 5.0 A·g^(-1))and cycling stability(268.3 mAh·g^(-1) after 100 cycles at 1.0 A·g^(-1)).Moreover,the rational preparation strategy for metal selenide-based heterostructure material presents a new way for high-performance SIB s.

关键词： Carbon nanofiber(CNF) Cobalt selenide(CoSe_(2)) Electrostatic spinning Sodium-ion storage

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Cobalt disulfide/carbon nanofibers with mesoporous heterostructure and excellent hydrophilicity for high energy density asymmetric supercapacitor

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Nano Research 2023年第7期16卷 10401-10411页

作者： Wenjie Liu fen qiao Jing Yang Jiaren Yuan Yi Xie Tao Wang Jinzhi Hu Jihua Zheng Rui Ren Xiaomin Kang Yan Zhao Jiangwei Zhang School of Energy&Power Engineering Jiangsu UniversityZhenjiang 212013China College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021China School of Physics and Materials Science Nanchang UniversityNanchang 330031China State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China Key Laboratory of Power Station Energy Transfer Conversion and System Ministry of EducationNorth China Electric Power UniversityBeijing 102206China

Herein,a unique mesoporous heterostructure(average pore size:15 nm)cobalt disulfide/carbon nanofibers(CoS_(2)/PCNFs)composite with excellent hydrophilicity(contact angle:23.5°)is prepared using polyethylene glycol(PEG)as a pore-forming agent.The CoS_(2)/PCNF electrode exhibits excellent cycle stability(95.2%of initial specific capacitance at 10 A·g^(-1)after 8000 cycles),good rate performance(46.5%at 10 A·g^(-1)),and high specific capacity(86.1 mAh·g^(-1)at 1 A·g^(-1),about 688.8 F·g^(-1)at 1 A·g^(-1)).Density functional theory(DFT)simulation elucidates that CoS_(2)tends to transfer substantial charges to CNF.As the center of positive charge,CoS_(2)is more likely to capture negative ions in the electrolyte,thus accelerating the ion diffusion process.The excellent properties of the electrode material can not only accelerate the electrochemical reaction kinetics,but also provide abundant redox-active sites and a high Faradaic capacity for the entire electrode due to the synergistic contributions of CoS_(2)nanoparticles,mesoporous heterostructure of PCNF,and admirable hydrophilicity of the composite material.A CoS_(2)/PCNF-0.25//AC(AC:activated carbon)asymmetric supercapacitor is assembled using CoS_(2)/PCNF-0.25 as the positive electrode and AC as the negative electrode,which possesses a high energy density(35.5 Wh·kg^(-1)at a power density of 824 W·kg^(-1))and superior cycling stability(maintaining over 98%of initial capacitance after 2000 cycles).In addition,the unique CoS_(2)/PCNF electrode is expected to be widely used in other electrochemical energy storage devices,such as lithium-ion batteries,sodium-ion batteries,lithium-sulfur batteries,etc.

关键词： supercapacitor cobalt disulfide carbon nanofibers porosity electrostatic spinning density functional theory(DFT)simulation

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A core-satellite structured type Ⅱ heterojunction photocatalyst with enhanced CO_(2) reduction under visible light

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Nano Research 2022年第10期15卷 8880-8889页

作者： Yuanyuan Cheng Yixian Liu Yunliang Liu Yaxi Li Ruqiang Wu Yongchao Du Najmeh Askari Naiyun Liu fen qiao Chenghua Sun Zhenhui Kang Haitao Li Institute for Energy Research School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang 212013China Faculty of Science Engineering&TechnologySwinburne University of TechnologyVictoria 3122Australia Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and DevicesSoochow UniversitySuzhou 215123China

Photocatalytic reduction of carbon dioxide into valuable chemicals is a sustainable and promising technology that alleviates the greenhouse effect and energy crisis.In this study,the Mn_(3)O_(4)/fenbO_(4) type Ⅱ heterojunction photocatalyst with a core-satellite structure was synthesized by the facile soft chemical method.The formation of a nano-heterojunction is supposed to effectively improve light capture,charge transfer,and interfacial charge separation in the photochemical reaction.Meanwhile,the heterojunction has a good ability to capture and activate CO_(2).Our results show that the prepared Mn_(3)O_(4)/fenbO_(4) photocatalyst exhibit obvious enhanced catalytic properties in the photocatalytic CO_(2) reduction reaction,where the CH_(4) yielding rate is 1.96 and 9.81 times those of fenbO_(4) and Mn_(3)O_(4),respectively.The transient photovoltage test(TPV)shows that the low frequency electrons are crucial to the effective transfer of photogenerated electrons and holes in the Mn_(3)O_(4)/fenbO_(4) nano heterojunctions.Analysis of in situ Fourier transform infrared spectroscopy(FTIR)verifies the effective CO_(2) adsorption on the Mn_(3)O_(4)/fenbO_(4) surface and the high selectivity of CH_(4) products.These properties of the Mn_(3)O_(4)/fenbO_(4) photocatalyst infer its broad prospects in the fields of carbon fixation and energy conservation.

关键词： typeⅡheterojunction Mn_(3)O_(4)/fenbO_(4) photocatalysis CO_(2)reduction

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