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Accelerating solar driven CO_(2) reduction via sulfur-doping boosted water dissociation and proton transfer

Nano Research 2024年第3期17卷 1056-1065页

作者： Ke Yan Liang Chen Yangguang hu Ting Wang Cong Chen chao Gao Youju huang Benxia Li School of Chemistry and Chemical Engineering Key Laboratory of Surface&Interface Science of Polymer Materials of Zhejiang ProvinceZhejiang Sci-Tech UniversityHangzhou 310018China College of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhou 311121China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China

Exploring efficient photocatalysts for solar driven CO_(2) reduction with water(h_(2)O)as a proton donor is highly imperative but remains a great challenge because the synchronous enhancement of CO_(2) activation,h_(2)O dissociation and proton transfer is hardly achieved on a ***,the sluggish h_(2)O dissociation impedes the photocatalytic CO_(2) reduction reaction involving multiple proton–electron coupling transfer ***,a sulfur-doped BiOCl(S-BiOCl)photocatalyst with abundant oxygen vacancies(OV)is developed,which exhibits broadband-light harvesting across solar spectrum and distinct photothermal effect due to *** photocatalytic CO_(2) reduction with h_(2)O in a gas–solid system,the high CO yield of 49.76μmol·g_(cat)^(-1)·h^(-1) with 100%selectivity is achieved over the S-BiOCl catalyst under a simulated *** h_(2)O-assisted CO_(2) reduction reaction on S-BiOCl catalyst is triggered by photocatalysis and the photothermal heating further enhances the reaction *** kinetic isotope experiments indicate that the sluggish h_(2)O dissociation affects the whole photocatalytic CO_(2) reduction *** presence of oxygen vacancies promotes the adsorption and activation of h_(2)O and CO_(2),and the doped S sites play a crucial role in boosting h_(2)O dissociation and accelerating the dynamic migration of hydrogen *** a result,the ingenious integration of OV defects,S sites and photothermal effect in S-BiOCl catalyst conjointly contributes to the significant improvement in photocatalytic CO_(2) reduction performance.

关键词： BiOCl sulfur doping photocatalytic CO_(2)reduction h_(2)O activation proton feeding

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Synergistically constructed lamination-like network of redox-active polyimide and MXene via π-π interactions for aqueous Nh_(4)^(+) storage

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Chinese Journal of Chemical Engineering 2024年第7期71卷 217-224页

作者： Jing he hongye Xuan Jing Jin Ke Yu Changyao Liyang Lintong hu Minjie Shi chao Yan School of Materials Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China Jiangsu New Yangzi Shipbuilding Co. LtdJingjiang 214532China

As a nonmetallic charge carrier,ammonium ion(Nh_(4)^(+))has garnered significant attention in the construction of aqueous batteries due to its advantages of low molar mass,small hydration size and rapid diffusion in aqueous *** are a kind of potential electro-active materials for aqueous Nh_(4)^(+)***,traditional polymer electrodes are typically created by covering the bulky collectors with excessive additives,which could lead to low volume capacity and unsatisfactory ***,a nanoparticle-like polyimide(PI)was synthesized and then combined with MXene nanosheets to synergistically construct an additive-free and self-standing PI@MXene composite ***,the redox-active PI nanoparticles are enclosed between conductive MXene flakes to create a 3D lamination-like network that promotes electron transmission,while theπ-πinteractions existing between PI and MXene contribute to the enhanced structural integrity and stability within the composite *** such,it delivers superior aqueous Nh_(4)^(+)storage behaviors in terms of a notable specific capacity of 110.7 mA·h·cm^(–3) and a long lifespan with only 0.0064%drop each ***,in-situ Raman and UV–Vis examinations provide evidence of reversible and stable redox mechanism of the PI@MXene composite electrode during Nh_(4)^(+)uptake/removal,highlighting its significance in the area of electrochemical energy storage.

关键词： Synergetic coupling Composite materials Polyimide Energy storage Aqueous ammonium ion batteries

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Plasmonic quantum dots modulated nano-mineral toward photothermal reduction of CO_(2)coupled with biomass conversion

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Nano Research 2024年第6期17卷 5061-5072页

作者： Guangbiao Cao haoran Xing haoguan Gui chao Yao Yinjuan Chen Yongsheng Chen Xiazhang Li National-local Joint Engineering Research Center of Biomass Refining and high-quality Utilization Changzhou UniversityChangzhou 213164China School of Civil and Environmental Engineering Georgia Institute of TechnologyAtlantaGA 30332-0373USA

Simultaneous conversion of CO_(2)and biomass into value-added chemicals through solar-driven catalysis holds tremendous importance for fostering a sustainable circular ***,plasmonic Bi quantum dots were immobilized on phosphoric acid modified attapulgite(P-ATP)nanorod using an in-situ reduction-deposition method,and were employed for photocatalytic reduction of CO_(2)coupled with oxidation of biomass-derived benzyl *** revealed that Bi atoms successfully integrated into the basal structure of P-ATP,forming chemically coordinated Bi-O-Si bonds that served as efficient transportation channels for *** incorporation of high-density monodispersed Bi quantum dots induced a surface plasmon resonance(SPR)effect,expanding the light absorption range into the near-infrared *** a consequence,the photo-thermal transformation was significantly accelerated,leading to enhanced reaction ***,50%Bi/P-ATP nanocomposite exhibited the highest plasmon-mediated photocatalytic Ch4 generation(115.7μmol·g^(−1)·h^(−1))and CO generation(44.9μmol·g^(−1)·h^(−1)),along with remarkable benzaldehyde generation rate of 79.5μmol·g^(−1)·h^(−1)in the photo-redox coupling system under solar light *** hydrogen protons released from the oxidation of benzyl alcohol facilitated the incorporation of more hydrogen protons into CO_(2)to form key Ch_(3)O−*** work demonstrates the synergistic solar-driven valorization of CO_(2)and biomass using natural mineral based catalyst.

关键词： photothermal catalysis clay mineral plasmon CO_(2)reduction biomass conversion

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highly selectiveα-C(sp^(3))-h arylation of alkenyl amides via nickel chain-walking catalysis

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Chinese Chemical Letters 2024年第7期35卷 271-275页

作者： haoran Shi Jiaxin Wang Yuqin Zhu hongyang Li Guodong Ju Lanlan Zhang chao Wang Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of ChemistryTianjin Normal UniversityTianjin 300387China

herein,we report the migratory hydroarylation of unactivated alkenes with aryl iodides using native and weakly coordinating amide directors under mild *** coordination of the monodentate directing group and the ligand enable the highly regioselective migratory hydroarylation via a chain walking process to form the thermodynamically stable five-membered nickelacyle *** protocol provides a variety of valuableα-aryl-substituted alkylamine products,and exhibited good functional group *** modification of bioactive compounds such as fenofibrate and indomethacin further highlights the synthetic value of this protocol.

关键词： Alkenes hydroarylation Chain-walking Regioselective Nickel catalysis

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Anchoring heterometallic cluster on P-doped carbon nitride for efficient photocatalytic nitrogen fixation in water and air ambient

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Chinese Chemical Letters 2024年第4期35卷 176-180页

作者： chao-Long Chen Rong Chen La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Light-driven nitrogen fixation to produce ammonia is a green and economical technology of nitrogen reduction but is still quite challenging, especially in an air atmosphere without any sacrificial ***, we demonstrate efficient photocatalytic nitrogen fixation using water and air directly by loading lanthanide–transition metal(4f–3d) cluster NdCo_(3) on two-dimensional P-doped graphitic carbon nitrides(PCN) material surface. Benefiting from the increase in the number of nitrogen vacancies(NVs) and highly matched band gap structure and excellent hole trapping ability of clusters, the NdCo_(3)/PCN photocatalyst exhibits efficient nitrogen reduction activity with 371(in air) and 825 μmol h^(-1)g^(-1)(in pure nitrogen)without any sacrificial reagents. The introduction of potassium sulfate inhibits hydrogen production and promotes nitrogen reduction activation. This work suggests that anchoring precisely structured clusters on 2D materials may enhance photocatalytic nitrogen reduction under normal temperature and pressure.

关键词： Photocatalytic Nitrogen fixation 4f-3d Cluster Air atmosphere

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Tailored heterostructured Ni_(3)N-NiO nano-frameworks for boosting electrocatalytic oxygen evolution via surface-modulated plasma strategy

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Nano Research 2024年第9期17卷 7909-7917页

作者： Bo Ouyang haonan Qin chao Sun Yilin Deng Ang Li Jipeng Zhu Erjun Kan Rajdeep Singh Rawat MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing School of ScienceNanjing University of Science&TechnologyNanjing 210094China The Laboratory of Road and Bridge Civil EngineeringSchool of ScienceNanjing University of Science&TechnologyNanjing 210094China Institute for Energy Research Jiangsu UniversityZhenjiang 212013China Natural Sciences and Science Education National Institute of EducationNanyang Technological University637616Singapore

The facile reconfiguration of phases plays a pivotal role in enhancing the electrocatalytic production of h2 through heterostructure *** chemical methods have been explored extensively for this purpose,plasma-based techniques offer a promising avenue for achieving heterostructured ***,the conventional plasma approach introduces complexities,leading to a multi-step fabrication process and challenges in precisely controlling partial surface structure modulation due to the intricate interaction *** our pursuit of heterostructures with optimized oxygen evolution reaction(OER)behavior,we have designed a facile auxiliary insulator-confined plasma system to directly attain a Ni_(3)N-NiO heterostructure(hNiNO).By meticulously controlling the surface heating process during plasma processing,such approach allows for the streamlined fabrication of hNiNO *** resulting nano-framework exhibits outstanding catalytic performance,as evidenced by its overpotential of 320 mV at a current density of 10 mA·cm^(-2),in an alkaline *** stands in stark contrast to the performance of NiO-covered Ni_(3)N fabricated using the conventional plasma method(sNiNO).Operando plasma diagnostics,coupled with numerical simulations,further substantiates the influence of surface heating due to auxiliary insulator confinement of the substrate on typical plasma parameters and the formation of the Ni_(3)N-NiO nanostructure,highlighting the pivotal role of controlled surface temperature in creating a high-performance heterostructured electrocatalyst.

关键词： structural modulation auxiliary insulator-confined plasma surface heating control heterostructure electrocatalytic O2 evolution

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Association of daily sitting time and leisure-time physical activity with body fat among ***

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Journal of Sport and health Science 2024年第2期13卷 195-203页

作者： Jingwen Liao Min hu Kellie Imm Clifton J.holmes Jie Zhu chao Cao Lin Yang Guangdong Provincial Key Laboratory of Physical Activity and health Promotion Guangzhou Sport UniversityGuangzhou 510500China Scientific Research Center Guangzhou Sport UniversityGuangzhou 510500China Division of Epidemiology&Genetics Department of Population and Public Health SciencesKeck School of Medicine of the University of Southern CaliforniaLos AngelesCA 90033USA Program in Physical Therapy Washington University School of MedicineSt.LouisMO 63110USA Center for human Nutrition Washington University School of MedicineSt.LouisMO 63110USA Department of Plastic and Reconstructive Surgery Shanghai East HospitalTongji UniversityShanghai 200070China Department of Cancer Epidemiology and Prevention Research Alberta Health ServicesCalgary T2S 3C3Canada Department of Oncology and Community health Sciences University of CalgaryCalgary T2N 1N4Canada

Background:Prolonged sitting and reduced physical activity lead to low energy ***,little is known about the joint impact of daily sitting time and physical activity on body fat *** investigated the independent and joint associations of daily sitting time and physical activity with body fat among ***:This was a cross-sectional analysis of *** representative data from the National health and Nutrition Examination Survey2011-2018 among adults aged 20 years or *** sitting time and leisure-time physical activity(LTPA)were self-reported using the Global Physical Activity *** fat(total and trunk fat percentage)was determined via dual X-ray ***:Among 10,808 adults,about 54.6%spent 6 h/day or more sitting;more than one-half reported no LTPA(inactive)or less than 150 min/week LTPA(insufficiently active)with only 43.3%reported 150 min/week or more LTPA(active)in the past *** fully adjusting for sociodemographic data,lifestyle behaviors,and chronic conditions,prolonged sitting time and low levels of LTPA were associated with higher total and trunk fat percentages in both *** stratifying by LTPA,the association between daily sitting time and body fat appeared to be stronger in those who were inactive/insuufficiently *** the joint analyses,inactive/insuufficiently active adults who reported sitting more than 8 h/day had the highest total(female:3.99%(95%confidence interval(95%CI):3.09%-4.88%);male:3.79%(95%CI:2.75%-4.82%))and trunk body fat percentages(female:4.21%(95%CI:3.09%-5.32%);male:4.07%(95%CI:2.95%-5.19%))when compared with those who were active and sitting less than 4 h/***:Prolonged daily sitting time was associated with increased body fat among *** higher body fat associated with 6 h/day sitting may not be offset by achieving recommended levels of physical activity.

关键词： Adults Body fat distribution Physical activity Sitting time

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Four New Terpyridine Complexes Based Polyoxometalates with[W_(10)O_(32)]^(4-) Anions as high-Efficiency Dual-Site Catalysis for Thioether Oxidation Reaction

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Chinese Journal of Chemistry 2024年第6期42卷 592-598页

作者： Yin Zhang Wei-Dong Yu Fang-Qian Wang Xiangnan Wang Jiawan Zhou chao Liu Jun Yan Junior Education Department Changsha Normal UniversityChangshaHunan410100 China School of Science Hunan University of Technology and BusinessChangshaHunan410000 China College of Chemistry and Chemical Engineering Central South UniversityChangshaHunan410000 China

Polyoxometalates modified with complex cations have attracted increasing attention because of the fascinating properties and the controllable *** adjusting the synthesis conditions,four new terpyridine complexes based hybrid POMs,[(TPY-h)CuCl]_(4)[W_(10)O_(32)]·2DMF·2h_(2)O(1),[(TPY-h)Cu(DMSO)(h_(2)O)]_(2)[W_(10)O_(32)]·2h_(2)O(2),[(TPY-h)_(2)Cu]_(2)[W_(10)O_(32)]·6DMSO·8h_(2)O(3) and[(TPY-Br)CuCl(DMSO)(h_(2)O)]_(2)[(TPY-Br)CuCl]_(2)[W_(10)O_(32)]·2DMSO·4h_(2)O(4),were prepared by using‘one-pot’***-crystal X-ray diffraction analyses,infrared radiation,etc.,revealed the structural composition of compounds 1—4,which indicates that synthesis conditions have a directional regulatory effect on the compounds *** oxidation catalytic reactions show 1—4 have good catalytic activities,and powder X-ray diffraction and thermogravimetry analysis show 1—4 have superduper catalytic ***,4 has better catalytic activity because of the different structure of terpyridine ***,a possible mechanism of dual-site catalysis by both cations and anions is proposed.

关键词： Polyoxometalates Terpyridine complexes Thioether oxidation Dual-site catalysis Clusters

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NaBh4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di han Yong-chao Zhang Qian Zhang Jin-Ting Wu Jian Gao Ji-Jun Zou Xiao-Dong Zhu State Key Laboratory Base of Eco-Chemical Engineering College of Chemical Engineering Qingdao University of Science and TechnologyQingdao266042China Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form h_(2)O_(2) in acidic medium has attracted extensive ***,the low activity,insufficient selectivity and high cost of catalysts have been the ***,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBh4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se *** cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOh and*O,which shows high activity,selectivity and long-term stability for acidic ORR to h_(2)O_(2).The onset potential is as low as 0.73 V *** hydrogen electrode(RhE),the h_(2)O_(2) selectivity is 84%(0 V ***),and the average electron transfer number is about ***,the h_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V ***,which presents high potential in electrocatalytic acidic ORR to h_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction hydrogen peroxide

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highly dispersive tetrahedral vanadium species on pure silica ZSM-12 zeolite boosting the selective oxidation of cyclohexane into cyclohexanone

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Science China Chemistry 2024年第7期67卷 2206-2214页

作者： Menglin Xie Ting Li chao Wu Xiaoling Liu Jinling Ni Siqin Yao Yu Zhou Shibo Xi Jun Wang State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China Institute of Sustainability for Chemicals Energy and Environment(ISCE2)Agency for ScienceTechnology and Research(A*STAR)Singapore 627833Republic of Singapore College of Materials Science and Engineering Sichuan UniversityChengdu 610065China

The selective oxidation of cyclohexane is a promising green route for the production of KA oil(cyclohexanol and cyclohexanone),but remains a huge challenge to design high-performing heterogeneous catalysts under mild ***,a pure silica ZSM-12(MTW topology)zeolite was applied as the support to immobilize highly dispersive tetrahedrally coordinated vanadium(V)species and the constructed catalyst 1%V/SZ-12 exhibited high efficiency in the fast and selective oxidation of cyclohexane into cyclohexanone with h_(2)O_(2).The reaction completed within 30 s,affording the selectivity of 99%towards cyclohexanone and the extremely high turnover frequency(TOF)of 5,891 h^(-1).1%V/SZ-12 was facilely reused with stable activity and feasibly extended to the oxidation of various cyclohexane *** one-dimensional 12-membered ring microchannels contributed to the formation and accessibility of tetrahedrally coordinated high valent V5+species as the robust active centers,which activated h_(2)O_(2) to generate V–O–O·,the active oxygen species for the electrophilic attack on cyclohexane to produce cyclohexanone as the sole product.

关键词： zeolite metal doping cyclohexane oxidation heterogeneous catalysis

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