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Understanding the oxidation chemistry of Ti_(3)C_(2)T_(x)(MXene)sheets and their catalytic performances

Journal of Energy Chemistry 2024年第1期88卷 437-445,I0010页

作者： Suvdanchimeg Sunderiya Selengesuren Suragtkhuu Solongo Purevdorj Tumentsereg Ochirkhuyag Munkhjargal Bat-Erdene Purevlkham Myagmarsereejid Ashley DSlattery Abdulaziz SRBati Joseph GShapter Dorj Odkhuu Sarangerel Davaasambuu Munkhbayar Batmunkh Department of Chemistry Division of Natural SciencesSchool of Arts and SciencesNational University of MongoliaUlaanbaatar 14200Mongolia queensland micro-and nanotechnology centre School of Environment and ScienceGriffith UniversityNathan campusBrisbaneQueensland 4111Australia Department of Physics Incheon National UniversityIncheon 22012Republic of Korea Australian Institute for Bioengineering and nanotechnology The University of QueenslandSt LuciaBrisbaneQueensland 4072Australia Adelaide microscopy The University of AdelaideAdelaideSouth Australia 5005Australia centre for Organic Photonics&Electronics School of Chemistry and Molecular BiosciencesThe University of QueenslandSt LuciaBrisbaneQueensland 4072Australia

Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and *** the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully ***,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several *** also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight *** results suggest that severely oxidized MXene could be a promising candidate for designing efficient *** to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.

关键词： 2D materials MXene Chemical degradation Catalysis Hydrogen evolution reaction

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Highly efficient nitrogen fixation over S-scheme heterojunction photocatalysts with enhanced active hydrogen supply

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National Science Review 2024年第5期11卷 315-325页

作者： Tong Bao Yamin Xi Chaoqi Zhang Peiyang Du Yitong Xiang Jiaxin Li Ling Yuan Chengzhong Yu Chao Liu School of Chemistry and Molecular Engineering East China Normal University Australian Institute for Bioengineering and nanotechnology The University of Queensland

Photocatalytic N2fixation is a promising strategy for ammonia（NH3） synthesis;however,it suffers from relatively low ammonia yield due to the difficulty in the design of photocatalysts with both high charge transfer efficiency and desirable N2adsorption/activation ***,an S-scheme CoSx/ZnS heterojunction with dual active sites is designed as an efficient N2fixation *** CoSx/ZnS heterojunction exhibits a unique pocket-like nanostructure with small ZnS nanocrystals adhered on a single-hole CoSxhollow *** the heterojunction,the ele ctronic interaction between ZnS and CoSxcreates electron-deficient Zn sites with enhanced N2chemisorption and electron-sufficient Co sites with active hydrogen supply for N2hydrogenation,cooperatively reducing the energy barrier for *** combination with the promoted photogenerated electron-hole separation of the S-scheme heterojunction and facilitated mass transfer by the pocket-like nanostructure,an excellent N2fixation performance with a high NH3yield of 1175.37 μmol g-1h-1is *** study provides new insights into the design of hetero junction photocatalysts for N2fixation.

关键词： photocatalysis nitrogen fixation S-scheme heterojunction active hydrogen ammonia

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Exploring the Roles of Single Atom in Hydrogen Peroxide Photosynthesis

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Nano-micro Letters 2024年第2期16卷 32-67页

作者： Kelin He Zimo Huang Chao Chen Chuntian Qiu Yu Lin Zhong Qitao Zhang International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518000China queensland micro‑and nanotechnology centre School of Environment and ScienceGriffith UniversityNathanQLD 4222Australia Institute for Sustainable Transformation School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 51006China ZJU‑Hangzhou Global Scientific and Technological Innovation Center Zhejiang UniversityHangzhou 311215China

This comprehensive review provides a deep exploration of the unique roles of single atom catalysts(SACs)in photocatalytic hydrogen peroxide(H_(2)O_(2))*** offer multiple benefits over traditional catalysts such as improved efficiency,selectivity,and flexibility due to their distinct electronic structure and unique *** review discusses the critical elements in the design of SACs,including the choice of metal atom,host material,and coordination environment,and how these elements impact the catalytic *** role of single atoms in photocatalytic H_(2)O_(2)production is also analysed,focusing on enhancing light absorption and charge generation,improving the migration and separation of charge carriers,and lowering the energy barrier of adsorption and activation of *** these advantages,several challenges,including H_(2)O_(2)decomposition,stability of SACs,unclear mechanism,and low selectivity,need to be *** towards the future,the review suggests promising research directions such as direct utilization of H_(2)O_(2),high-throughput synthesis and screening,the creation of dual active sites,and employing density functional theory for investigating the mechanisms of SACs in H_(2)O_(2)*** review provides valuable insights into the potential of single atom catalysts for advancing the field of photocatalytic H_(2)O_(2)production.

关键词： Single atom catalysts H_(2)O_(2)photosynthesis Catalyst design and optimization

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Reducing the vacancies associated with ferroelectric polarization to promote photocatalytic overall water splitting

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Science China Chemistry 2024年第10期67卷 3258-3264页

作者： Haozhi Qi Yuyang Kang Jian-An Liu Lichang Yin Wenyu Zhang Shangyi Ma Jianhang Qiu Lingli Li Weijin Hu Lianzhou Wang Gang Liu Institute of Metal Research Chinese Academy of SciencesShenyang 110016China School of Materials Science and Engineering University of Science and Technology of ChinaShenyang 110016China Nanomaterials centre School of Chemical Engineering and Australian Institute for Bioengineering and NanotechnologyThe University of QueenslandSt LuciaBrisbane QLD 4072Australia

Ferroelectric materials hold great promise in photocatalytic water splitting because their built-in electric field induced by the depolarization field can fulfill the separation of photogenerated ***,a number of intrinsic charged vacancy defects are simultaneously generated to screen the depolarized field for stabilizing the crystal structure,always resulting in severe recombination of photogenerated carriers and thus poor overall water splitting ***,we proposed a strategy to promote the separation and transport of photogenerated carriers of ferroelectric photocatalysts by adjusting the ferroelectric polarization and altering the coordination environment of elements to reduce the defect ***,we prepared a series of Ta-doped PbTiO_(3)with low Pb(V_(Pb))and O(V_(O))vacancy concentrations by reducing the polarization intensity and strengthening the Pb–O *** Ta-doped PbTiO_(3)shows efficient charge separation and greatly enhanced photocatalytic overall water splitting activity with the assistance of *** work highlights the importance of regulating ferroelectric polarization and vacancy defect concentration by the doping strategy in charge separation for photocatalytic water splitting.

关键词： PbTiO_(3) ferroelectric polarization vacancy defect element doping photocatalytic overall water splitting

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Enhancing performance and longevity of solid-state zinc-iodine batteries with fluorine-rich solid electrolyte interphase

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Materials Futures 2024年第3期3卷 121-131页

作者： Yongxin Huang Yiqing Wang Xiyue Peng Tongen Lin Xia Huang Norah S Alghamdi Masud Rana Peng Chen Cheng Zhang Andrew K Whittaker Lianzhou Wang and Bin Luo Australian Institute for Bioengineering and nanotechnology(AIBN) The University of QueenslandBrisbaneQLD4072Australia School of Chemical Engineering The University of QueenslandBrisbaneQLD4072Australia School of Chemistry and Molecular Biosciences Faculty of ScienceThe University of QueenslandBrisbaneQLD4072Australia Department of Chemistry Faculty of ScienceImam Mohammad Ibn Saud Islamic University(IMSIU)Riyadh 11564Saudi Arabia

Rechargeable zinc-iodine(ZnI_(2))batteries have gained popularity within the realm of aqueous batteries due to their inherent advantages,including natural abundance,intrinsic safety,and high theoretical ***,challenges persist in their practical applications,notably battery swelling and vulnerability in aqueous electrolytes,primarily linked to the hydrogen evolution reaction and zinc dendrite *** address these challenges,this study presents an innovative approach by designing a solid-state ZnI_(2)battery featuring a solid perfluoropolyether based polymer *** results demonstrate the formation of a solid electrolyte interphase layer on zinc,promoting horizontal zinc growth,mitigating dendrite penetration,and enhancing battery cycle ***,the solid electrolyte hinders the iodine ion shuttle effect,reducing zinc foil *** batteries employing this electrolyte demonstrate excellent cycle performance,maintaining stability for approximately 5000 h at room temperature,while solid-state ZnI_(2)batteries exhibit over 7000 cycles with a capacity retention exceeding 72.2%.This work offers a promising pathway to achieving reliable energy storage in solid-state ZnI_(2)batteries and introduces innovative concepts for flexible and wearable zinc batteries.

关键词： zinc-iodine battery solid electrolyte zinc metal anode electrolyte interphase shuttle effect

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Organic ligand nanoarchitectonics for BiVO_(4) photoanodes surface passivation and cocatalyst grafting

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Nano Research 2024年第5期17卷 3667-3674页

作者： Jingyi Lin Xin Li Zhiliang Wang Runlu Liu Hui Pan Yixin Zhao Lingti Kong Yao Li Shenmin Zhu Lianzhou Wang State Key Laboratory of Metal Matrix Composites School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Nanomaterials centre School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnologythe University of QueenslandQLD 4072Australia School of Environmental Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China Hubei Key Laboratory of Plasma Chemistry and Advanced Materials Wuhan Institute of TechnologyWuhan 430205China

Bismuth vanadate(BiVO_(4))is a promising photoanode material for efficient photoelectrochemical(PEC)water splitting,whereas its performance is inhibited by detrimental surface *** solve the problem,herein,a low-cost organic molecule 1,3,5-benzenetricarboxylic acid(BTC)is selected for surface passivation of BiVO_(4) photoanodes(BVOs),which also provides bonding sites for Co^(2+)to anchor,resulting in a Co-BTC-BVO *** to its strong coordination with metal ions,BTC not only passivates surface states of BVO,but also provides bonding between BVO and catalytic active sites(Co^(2+))to form a molecular *** study and interfacial charge kinetic investigation reveal that chemical bonding formed at the interface greatly suppresses charge recombination and accelerates charge *** obtained Co-BTC-BVO photoanode exhibits a photocurrent density of 4.82 mA/cm^(2) at 1.23 V *** hydrogen electrode(RHE)and a low onset potential of 0.22 VRHE under AM 1.5 G illumination,which ranks among the best photoanodes coupled with Co-based *** work presents a novel selection of passivation layers and emphasizes the significance of interfacial chemical bonding for the construction of efficient photoanodes.

关键词： bismuth vanadate photoanode water splitting surface passivation bridging ligands

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Nitrogen incorporated oxygen vacancy enriched MnCo_(2)O_(x)/BiVO_(4) photoanodes for efficient and stable photoelectrochemical water splitting

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Nano Research 2024年第3期17卷 1140-1150页

作者： Liangcheng Xu Yingjuan Zhang Boyan Liu Xin Wang Gangqiang Zhu Lianzhou Wang Songcan Wang Wei Huang Frontiers Science Center for Flexible Electronics Xi’an Institute of Flexible Electronics(IFE)Northwestern Polytechnical University127 West Youyi RoadXi’an 710072China School of Physics and Information Technology Shaanxi Normal UniversityXi’an 710062China Nanomaterials centre Australian Institute for Bioengineering and Nanotechnology and School of Chemical EngineeringThe University of QueenslandBrisbaneQueensland 4072Australia Research&Development Institute of Northwestern Polytechnical University in Shenzhen Sanhang Science&Technology BuildingNo.45thGaoxin South 9th RoadNanshan DistrictShenzhen 518063China

Oxygen vacancies in oxygen evolution cocatalysts(OECs)can significantly improve the photoelectrochemical(PEC)water splitting performance of ***,OECs with abundant oxygen vacancies have a poor stability when exposing to the highly-oxidizing photogenerated ***,we partly fill oxygen vacancies in a MnCo_(2)O_(x) OEC with N atoms by a combined electrodeposition and sol-gel method,which dramatically improves both photocurrent density and stability of a BiVO_(4) *** optimized N filled oxygen vacancy-rich MnCo_(2)O_(x)/BiVO_(4) photoanode(3 at.%of N)exhibits an outstanding photocurrent density of 6.5 mA·cm^(-2) at 1.23 VRHE under AM 1.5 G illumination(100 mW·cm^(-2)),and an excellent stability of over 150 *** characterizations and theoretical calculations demonstrate that N atoms stabilize the defect structure and modulate the surface electron distribution,which significantly enhances the stability and further increases the photocurrent ***,other heteroatoms such as carbon,phosphorus,and sulfur are confirmed to have similar effects on improving PEC water splitting performance of photoanodes.

关键词： water splitting oxygen evolution bismuth vanadate(BiVO_(4)) filling oxygen vacancies cocatalysts

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Approaching Ultimate Synthesis Reaction Rate of Ni-Rich Layered Cathodes for Lithium-Ion Batteries

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Nano-micro Letters 2024年第10期16卷 392-402页

作者： Zhedong Liu Jingchao Zhang Jiawei Luo Zhaoxin Guo Haoran Jiang Zekun Li Yuhang Liu Zijing Song Rui Liu Wei-Di Liu Wenbin Hu Yanan Chen School of Materials Science and Engineering Tianjin UniversityTianjin 300072People's Republic of China School of Materials Science and Engineering Shandong University of Science and TechnologyQingdao 266590People's Republic of China Australian Institute of Bioengineering and nanotechnology The University of QueenslandSt LuciaQLD 4072Australia

Nickel-rich layered oxide LiNi_(x)Co_(y)MnzO_(2)(NCM,x+y+z=1)is the most promising cathode material for high-energy lithium-ion ***,conventional synthesis methods are limited by the slow heating rate,sluggish reaction dynamics,high energy consumption,and long reaction *** overcome these chal-lenges,we first employed a high-temperature shock(HTS)strategy for fast synthesis of the NCM,and the approaching ultimate reaction rate of solid phase transition is deeply investigated for the first *** the HTS process,ultrafast average reaction rate of phase transition from Ni_(0.6)Co_(0.2)Mn_(0.2)(OH)_(2) to Li-containing oxides is 66.7(%s^(-1)),that is,taking only 1.5 *** ultrahigh heating rate leads to fast reaction kinetics,which induces the rapid phase transition of NCM *** HTS-synthesized nickel-rich layered oxides perform good cycling performances(94%for NCM523,94%for NCM622,and 80%for NCM811 after 200 cycles at 4.3 V).These findings might also assist to pave the way for preparing effectively Ni-rich layered oxides for lithium-ion batteries.

关键词： Nickel-rich layered oxides High-temperature shock Solid reaction kinetics Phase transition Reaction rate

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Superconducting joints using reacted multifilament MgB_(2)wires:A technology toward cryogen-free MRI magnets

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Journal of Magnesium and Alloys 2024年第1期12卷 159-170页

作者： Dipak Patel Akiyoshi Matsumoto Hiroaki Kumakura Yuka Hara Toru Hara Minoru Maeda Hao Liang Yusuke Yamauchi Seyong Choi Jung Ho Kim Md Shahriar A.Hossain School of Mechanical and Mining Engineering The University of QueenslandSt LuciaQueensland 4072Australia National Institute for Materials Science(NIMS) 1-2-1 SengenTsukubaIbaraki 305-0047Japan Department of Electrical Engineering and Kangwon High Magnetic Field Center Institute of Quantum Convergence TechnologyKangwon National UniversityGangwon 24341Republic of Korea Australian Institute for Bioengineering and nanotechnology(AIBN) The University of QueenslandSt LuciaQueensland 4072Australia Department of Materials Process Engineering Graduate School of EngineeringNagoya UniversityNagoyaAichi 464-8603Japan Institute for Superconducting and Electronic Materials Australian Institute for Innovative MaterialsUniversity of WollongongNorth WollongongNew South Wales 2500Australia

The development of superconducting joining technology for reacted magnesium diboride(MgB_(2))conductors remains a critical challenge for the advancement of cryogen-free MgB_(2)-based magnets for magnetic resonance imaging(MRI).Herein,the fabrication of superconducting joints using reacted carbon-doped multifilament MgB_(2)wires for MRI magnets is *** achieve successful superconducting joints,the powder-in-mold method was employed,which involved tuning the filament protection mechanism,the powder compaction pressure,and the heat treatment *** fabricated joints demonstrated clear superconducting-to-normal transitions in self-field,with effective magnetic field screening up to 0.5 T at 20 *** evaluate the interface between one of the MgB_(2)filaments and the MgB_(2)bulk within the joint,serial sectioning was conducted for the first time in this type of superconducting *** serial sectioning revealed space formation at the interface,potentially caused by the volume shrinkage associated with the MgB_(2)formation or the combined effect of the volume shrinkage and the different thermal expansion coefficients of the MgB_(2)bulk,the filament,the mold,and the sealing *** findings are expected to be pivotal in developing MgB_(2)superconducting joining technology for MRI magnet applications through interface engineering.

关键词： Mg B2 superconducting joint MgB_(2)conductor MRI applications Cryogen-free magnet Persistent-mode operation

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Heterocyclic Molecules Tethered Branched Polymers with Innate Immune Stimulating Activity

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CCS Chemistry 2024年第5期6卷 1278-1288页

作者： Jiayu Zhao Liping Liu Yibo Wang Zichao Huang Yu Zhang Ruirui Qiao Thomas P.Davis Zhaohui Tang Wantong Song Xuesi Chen Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022 School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026 Laboratory of Chemical Biology Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022 Jilin Biomedical Polymers Engineering Laboratory Changchun 130022 Australian Institute of Bioengineering and nanotechnology The University of QueenslandBrisbaneQueensland 4072

We report herein an interesting finding that heterocyclic molecules tethered branched polymers exhibit innate immune stimulating *** we conjugated a series of five-,six-,or seven-membered heterocyclic molecules to branched polyethylenimine(bPEI),over 70%of them could induce the secretion of interferon-β(IFN-β)from murine dendritic and human leukemia monocytic(DC2.4 and THP-1)cells through activating the stimulator of interferon genes(STING)*** further proved that this kind of innate stimulating activity was dependent on the macromolecular architecture as heterocyclic molecules tethered linear PEI(lPEI)or dendritic polyamidoamine(PAMAM)induced no or much less IFN-β***,we prepared a series of poly-L-lysine(PLL)-derivatives with different branches to tether with heterocyclic molecules and proved that this kind of bPEI-like structure was important in en hancing the binding affinity with STING proteins and for exhibiting innate stimulating activity.

关键词： bioactive materials polymers heterocycles branched structure immunity

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