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Single-atom catalysis for advanced oxidation and reduction systems in water decontamination

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Rare Metals 2024年第8期43卷 3576-3606页

作者： Jie Teng Jin-Hui Xu Wen-Xin Sun xue-Feng liu Xia Xu Guo-Shuai liu School of Urban Construction Changzhou UniversityChangzhou 213164China School of Environmental and Civil Engineering Jiangnan UniversityWuxi 214122China

Water scarcity is an escalating global crisis,posing a severe threat to populations ***,exploring various materials to remove emerging contaminants from freshwater sources has garnered significant *** this regard,single-atom catalysis(SACs) has emerged as a catalyst of scientific progress in water purification and treatment methodologies during recent *** exhibit exceptional catalytic activity,selectivity and stability,due to their near-perfect atom utilization,highly unsaturated coordination environment and uniform reaction ***,a comprehensive and critical review encompassing the successful integration of SACs into water purification processes needs to be *** review aims to accentuate recent trends by presenting the synthesis,structure,and environment and energy application-relevant properties of *** results show that a comprehensive and multi-perspective summary of the advantages of SACs in environmental remediation can have significant benefits,such as fast kinetics,costeffectiveness,*** oxidation and reduction processes of SACs and functional SACs materials in water purification were ***,the last section is devoted to the current research gaps and further perspectives on the application of SACs in water treatment,which are summarized and analyzed.

关键词： Single-atom catalysis Water treatment Oxidation Reduction

Boosting ammonia production in electrocatalytic NO_(x)reduction on a robust Fe/FeMoO_(4)catalyst

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Nano Research 2024年第7期17卷 5801-5806页

作者： Dong-xue liu Xin Deng Yong-Fu Zhu Zhe Meng xue-Feng Sun Miao-Miao Shi Hai-Xia Zhong Jun-Min Yan Key Laboratory of Automobile Materials Ministry of EducationSchool of Materials Science and EngineeringJilin UniversityChangchun 130022China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Electrocatalytic reduction of nitrate(NO_(3)^(−))and nitride(NO_(2)^(−))to ammonia(NH3)is of wide interest as a promising alternative to the energy-intensive Haber-Bosch route for mitigating the vast energy consumption and the accompanied carbon dioxide emission,as well as benefiting for the relevant sewage ***,exploring an efficient and low-cost catalyst with high atomic utilization that can effectively facilitate the slow multi-electron transfer process remains a grand ***,we present an efficient hydrogenation of NO_(3)^(−)/NO_(2)^(−)species to NH3 in both alkaline and neutral environments over the Fe_(2)(MoO_(4))_(3)derived hybrid electrocatalyst with the metallic Fe site on FeMoO_(4)(Fe/FeMoO_(4)).The Mo ingredient can play a synergistically positive role in further promoting the NH_(3) production on *** a result,Fe/FeMoO_(4)behaves well in the electrochemical NH_(3) generation from NO_(2)^(−)with a maximum NH_(3) Faradaic efficiency(FE)of 96.53%and 87.68%in alkaline and neutral electrolyte,corresponding to the NH_(3) yield rate of 640.68 and 302.56 mg·h^(−1)·mg_(cat.)^(−1),respectively,which outperforms the Fe and Mo counterpart and other similar catalyst,showing the robust catalytic capacity of each active site.

关键词： ammonia synthesis NO_(x)reduction synergistic effect alkaline/neutral electrolyte

Light-driven sextuple theranostics:nanomedicine involving second near-infrared AIE-active Ir(Ⅲ)complex for prominent cancer treatment

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Science China Chemistry 2024年第7期67卷 2314-2324页

作者： xue liu Jiangao Li Fei Zhang Dingyuan Yan Lei Wang Dong Wang Ben Zhong Tang Center for AIE Research Shenzhen Key Laboratory of Polymer Science and TechnologyGuangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Material Science and EngineeringShenzhen UniversityShenzhen 518060China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen 518060China School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhen(CUHK-Shenzhen)Shenzhen 518172China

Light-driven cancer theranostics has shown inexhaustible and vigorous vitality by virtue of its high efficacy,prominent controllability and *** of an all-round theranostic material simultaneously affording both multimodal diagnosis imaging and synergistic phototherapy would be an appealing yet significantly challenging ***,a novel nanomedicine Ir@PPEG-MeEPO was ingeniously constructed by integrating beforehand1O2-charged amphiphilic polymer and well-tailored Ir(Ⅲ)complex IrDPTP,which was featured by second near-infrared(NIR-Ⅱ)aggregation-induced emission(AIE)tendency,efficient reactive oxygen species(ROS)generation,good photothermal conversion efficiency and high-performance hydrogen gas *** the best of our knowledge,IrDPTP held the longest emission wavelength among all reported AIE Ir(Ⅲ)***,Ir@PPEG-MeEPO was capable of controllably releasing ROS via triggered photothermal effect upon NIR irradiation,making it well-adapted to hypoxic environment of *** distinctive characteristics of Ir@PPEG-MeEPO endowed it with unprecedented performance on sextuple theranostics comprised of NIR-Ⅱfluorescence-photoacoustic-photothermal trimodal imaging and photodynamic-photothermal-hydrogen trimodal therapy,witnessed by the precise tumor diagnosis and complete tumor *** study would open up new perspectives for the exploration of superior nanomedicine for practical cancer theranostics.

关键词： aggregation-induced emission NIR-II emission cancer theranostics multimodal diagnosis imaging multimodal therapy

Unraveling role of double-exchange interaction in electrochemical water oxidation by external magnetic field

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Rare Metals 2024年第1期43卷 289-297页

作者： Jun Li Jun-Ming Li Hong Hong Dong-xue liu Qing-Qi Cao Dun-Hui Wang National Laboratory of Solid State Microstructures and Jiangsu Provincial Key Laboratory for Nanotechnology Nanjing UniversityNanjing 210093China School of Electronics and Information Hangzhou Dianzi UniversityHangzhou 310018China

Double-exchange(DE) interaction plays an important role in electrocatalytic oxygen evolution reaction(OER).However,precise achievement of DE interaction often requires foreign dopants or vacancy engineering,leading to destabilization of the catalysts and deterioration of *** contrast,the utilization of environmentally friendly,contactless,and continuously adjustable magnetic fields to study the OER process is profitable to avoid aforementioned interference factors and further elucidate the direct relationship_(0.5)between DE interaction and OER ***,by using cobalt hydroxide carbonate(Co(OH)(CO_(3))·xH_(2)O,CoHC) nanostructures as a proof-of-concept study,external magnetic fields are carefully implemented to verify the role of DE interaction during water oxidation *** studies reveal that external magnetic fields effectively enhance the reaction rate of the catalyst,the overpotential decreases from 386 to 355 mV(100 mA·cm^(-2)),while Tafel slopes drastically decline from 93 to 67 mV·dec^(-1)(1.0 T).Moreover,magnetic field increment exhibits robust *** in situ Raman and impedance measurements under external field,it can be found that magnetic field promotes the electron migration between Co^(2+) and Co^(3+) in the CoHC catalysts with the assistance of DE interactions,thus boosting the OER efficiency.

关键词： Magnetic field Double-exchange(DE)interaction Electrocatalysis Oxygen evolution reaction(OER) Cobalt hydroxide carbonate

MOF‐derived 1D/3D N‐doped porous carbon for spatially confined electrochemical CO2 reduction to adjustable syngas

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Carbon Energy 2024年第8期6卷 1-13页

作者： Wei Zhang Hui Li Daming Feng Chenglin Wu Chenghua Sun Baohua Jia xue liu Tianyi Ma Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials Institute of Clean Energy ChemistryCollege of ChemistryLiaoning UniversityShenyangLiaoningChina School of Science RMIT UniversityMelbourneVictoriaAustralia School of Pharmaceutical and Chemical Engineering Taizhou UniversityTaizhouZhejiangChina Department of Chemistry and Biotechnology Swinburne University of TechnologyHawthornVictoriaAustralia

Electrochemical reduction of CO_(2)to syngas(CO and H_(2))offers an efficient way to mitigate carbon emissions and store intermittent renewable energy in ***,the hierarchical one‐dimensional/three‐dimensional nitrogen‐doped porous carbon(1D/3D NPC)is prepared by carbonizing the composite of Zn‐MOF‐74 crystals in situ grown on a commercial melamine sponge(MS),for electrochemical CO_(2)reduction reaction(CO_(2)RR).The 1D/3D NPC exhibits a high CO/H_(2)ratio(5.06)and CO yield(31 mmol g^(−1)h^(−1))at−0.55 V,which are 13.7 times and 21.4 times those of 1D porous carbon(derived from Zn‐MOF‐74)and N‐doped carbon(carbonized by MS),*** is attributed to the unique spatial environment of 1D/3D NPC,which increases the adsorption capacity of CO_(2)and promotes electron transfer from the 3D N‐doped carbon framework to 1D carbon,improving the reaction kinetics of CO_(2)*** results and charge density difference plots indicate that the active site of CO_(2)RR is the positively charged carbon atom adjacent to graphitic N on 1D carbon and the active site of HER is the pyridinic N on 1D *** presence of pyridinic N and pyrrolic N reduces the number of electron transfer,decreasing the reaction kinetics and the activity of CO_(2)*** CO/H_(2)ratio is related to the distribution of N species and the specific surface area,which are determined by the degree of spatial confinement *** CO/H_(2)ratios can be regulated by adjusting the carbonization temperature to adjust the degree of spatial confinement *** the low cost of feedstock and easy strategy,1D/3D NPC catalysts have great potential for industrial application.

关键词： electrochemical CO_(2)reduction reaction melamine sponge metal‐organic frameworks porous carbon syngas

Characterization of high intensity ultrasound on structure， digestibility， and IgG binding capacity of Pacific oyster(Crassostrea gigas) tropomyosin

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Food Science and Human Wellness 2024年

作者： Li liu xue liu Yuyang Ma Mingyong Zeng College of Food Science and Engineering， Ocean University of China Qingdao Engineering Research Center for Preservation Technology of Marine Foods

In this study， the different powers (100-500 W) of high intensity ultrasound (HIU) were configured to investigate the mechanism of action on the tropomyosin (TM) structure， IgG binding capacity and digestive properties in oyster. The α-helix content of the HIU-treated TM decreased from 75.3% (control) to 41.8% (500 W) with the conversion of α-helix to random coil in TM molecules. The tertiary structure was changed with the decrease of particle size (from 165.5 to 85.6 nm) and the variety in aggregation state. Remarkably， the IgG binding capacity of TM decreased resulting from the higher power HIU treatment (300-500 W). After gastrointestinal digestion， the binding capacity of TM to IgG decreased to 1.31 with 500 W treatment， while the digestibility significantly increased. Overall， the present study suggested that the HIU-induced structural changes contributed to improving in vitro digestibility and reducing IgG binding capacity. This study contributes significant potential in terms of oyster allergen reduction.

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Hematuria after nocturnal exercise of a man: A case report

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World Journal of Clinical Cases 2024年第5期12卷 1025-1028页

作者： Ming-Jian Bai Song-Tao Yang xue-Kai liu Department of Clinical Laboratory Aerospace Center HospitalBeijing 100049China Department of Nephrology Aerospace Center HospitalBeijing 100049China

BACKGROUND A man experienced multiple episodes of macroscopic hematuria following nocturnal *** stones and tumors were considered the two most likely *** patient had two hobbies:Consuming health care products in large quantities and engaging in late-night *** SUMMARY Health care products contain a large amount of calcium phosphate,and we hypothesize that this could induce the formation of small phosphate *** exercise,the urinary system is abraded,resulting in *** patient was advised to stop using the health care ***,the aforementioned symptoms disappeared ***,the patient resumed the above two habits one year later;correspondingly,the macroscopic hematuria *** This finding further confirmed the above inference and allowed for a new avenue to determine the cause of the patient’s hematuria.

关键词： Hematuria Health care products Exercise Case report

Acceptor-engineering tailored type-Ⅰ photosensitizer with aggregation-induced NIR-II emission for cancer multimodal phototheranostics

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Science China Chemistry 2024年第8期67卷 2647-2660页

作者： Jiangao Li Niu Niu Deliang Wang xue liu Yi Qin Lei Wang Ben Zhong Tang Dong Wang Center for AIE Research Shenzhen Key Laboratory of Polymer Science and TechnologyGuangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China Guangzhou Municipal and Guangdong Provincial Key Laboratory of Molecular Target Clinical Pharmacologythe State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical Sciences and the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhou 511436China School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhen(CUHK-Shenzhen)Shenzhen 518172China

Exploration of single molecular species synchronously featured by long excitation/emission wavelength, accurate diagnosis, and effective therapy, remains supremely appealing to implement high-performance cancer phototheranostics. However, those previously established phototheranostic agents are undiversified and stereotyped in terms of structural skeleton, and generally exhibit insufficient phototheranostic outcomes. Herein, we innovatively utilized indanone-condensed thiadiazolo[3,4-g]quinoxaline(ITQ) as electron acceptor to construct novel photosensitizer with second near-infrared(NIR-II) emission. Experimental study and theoretical calculation demonstrated that comparing with the counterparts constituting by widely employed NIR-II building block benzobisthiadiazole(BBTD) and 6,7-diphenylthiadiazoloquinoxaline(DPTQ), ITQ-based photosensitizer(TITQ) showed superior aggregation-induced emission(AIE) characteristics, much stronger type-I reactive oxygen species(ROS) production, and prominent photothermal conversion capacity. Furthermore, TITQ nanoparticles with excellent biocompatibility were capable of effectively accumulating in the tumor site and visualizing tumor through fluorescence-photoacoustic-photothermal trimodal imaging with highly spatiotemporal resolution, and completely eliminating tumor by type-I photodynamic-photothermal therapy.

关键词： phototheranostics aggregation-induced emission NIR-Ⅱfluorescence acceptor engineering photodynamic-photothermal therapy

Recent Advances in the Electrochemical Defluorinative Transformations of C-F Bonds

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Chinese Journal of Chemistry 2024年第16期42卷 1913-1928页

作者： Qinhui Wan Rui-xue liu Zhongyi Zhang Xia-Die Wu Zhong-Wei Hou Lei Wang Advanced Research Institute and Schoolof Pharmaceutical Sciences Taizhou UniversityJiaojiangZhejiang 318000China Department of Chemistry Southern University of Science and TechnologyhenzhenGuangdong 518055China College of Material Chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistry and Material Technology Ministryof EducationHangzhou Normal UniversityHangzhouZhejiang 311121China

Organic fluorine compounds are ubiquitous and pivotally important organic molecules,yet their activation and transformation have long been a formidable challenge due to the high energy and low reactivity of C-F *** electrosynthesis,an environmentally benign synthetic method in organic chemistry,enables a myriad of chemical transformations without the need for external redox *** recent years,organic electrochemistry has emerged as a powerful tool for achieving the activation and transformation of C-F bonds in fluorine-containing *** review aims to succinctly recapitulate the latest advancements in the electrochemical defluorinative transformations of C-F bonds and to delve into the reaction design,mechanistic insights,and developmental prospects ofthese methods.

关键词： Organic electrochemistry Electroreduction Defluorination C-F bond activation Organic fluorine compounds