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Modulating eg orbitals through ligand engineering to boost the electrocatalytic activity of NiSe for advanced lithium-sulfur batteries

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Journal of Energy Chemistry 2022年第11期31卷 317-323,I0009页

作者： Tianran Yan Jie Feng Pan Zeng Gang Zhao Lei Wang Cheng Yuan Chen Cheng Youyong Li Liang Zhang Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123JiangsuChina Jiangsu Key Laboratory for Carbon-Based Functional Materials&Devices Soochow UniversitySuzhou 215123JiangsuChina Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123JiangsuChina

Accelerating the sluggish redox kinetics of lithium polysulfides(LiPSs)by electrocatalysis is essential to achieve high performance lithium-sulfur(Li-S)***,the issue of insufficient catalytic activity remains to be ***,a strategy of modulating e_(g) orbitals through ligand engineering has been proposed to boost the catalytic activity of NiSe for rapid LiPSs redox *** X-ray spectroscopic measurements and theoretical calculations reveal that partial substitution of Se with N disrupts the octahedral coordination of Ni atoms in NiSe,leading to the reduced degeneracy and upward shift of e_(g) orbitals of Ni 3 d *** a consequence,the bonding strength of N-substituted NiSe(N-NiSe)with LiPSs is enhanced,which facilitates the interfacial charge transfer kinetics and accelerates the LiPSs redox ***,the Li-S batteries assembled with N-NiSe present a high capacity of 682.6 mAh g^(-1) at a high rate of 5 C and a high areal capacity of 6.5 mAh cm^(-2)at a high sulfur loading of 6 mg cm^(-2).This work provides a promising strategy to develop efficient transition-metal based electrocatalysts for Li-S batteries through e_(g) orbital modulation.

关键词： Li-S batteries eg orbitals modulation Ligand engineering Shuttle effect Redox kinetics

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In-situ transient photovoltage study on interface electron transfer regulation of carbon dots/NiCo_(2)O_(4) photocatalyst for the enhanced overall water splitting activity

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Nano Research 2022年第3期15卷 1786-1795页

作者： Haodong Nie Yan Liu Yi Li Kaiqiang Wei Zhenyu Wu Hong Shi Hui Huang Yang Liu Mingwang Shao Zhenhui Kang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Macao Institute of Materials Science and Engineering Macao University of Science and TechnologyTaipa 999078Macao SARChina

Photocatalytic hydrogen production by overall water solar-splitting is a prospective strategy to solve energy ***,the rapid recombination of photogenerated electron–hole pairs deeply restricts photocatalytic activity of ***,the in-situ transient photovoltage(TPV)technique was developed to investigate the interfacial photogenerated carrier extraction,photogenerated carrier recombination and the interfacial electron delivery kinetics of the *** carbon dots/NiCo_(2)O_(4)(CDs/NiCo_(2)O_(4))composite shows weakened recombination rate of photogenerated carriers due to charge storage of CDs,which enhances the photocatalytic water decomposition activity without any *** can accelerate the interface electron extraction about 0.09 ms,while the maximum electron storage time by CDs is up to 0.7 *** optimal CDs/NiCo_(2)O_(4)composite(5 wt.%CDs)displays the hydrogen production of 62µmol·h^(−1)·g^(−1) and oxygen production of 29µmol·h^(−1)·g^(−1) at normal atmosphere,which is about 4 times greater than that of pristine NiCo_(2)O_(4).This work provides sufficient evidence on the charge storage of CDs and the interfacial charge kinetics of photocatalysts on the basis of in-situ TPV tests.

关键词： carbon dots photocatalytic hydrogen evolution transient photovoltage technique normal pressure continuous wavelet analysis

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Multi-site anchoring lead-halide octahedral by benzylphosphonic acid to regulate phase distribution for efficient PeLEDs

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Nano Research 2024年第11期17卷 10034-10041页

作者： Jiahao Tang Yifei Wang Hengyang Xiang Run Wang Kun Zhang Xinyi Lv Xinrui Chen Ziqing Xu Zhesheng Chen Lei Wang Aidi Zhang An Xie Haibo Zeng MIIT Key Laboratory of Advanced Display Materials and Devices Institute of Optoelectronics and Nanomaterials College of Materials Science and Engineering Nanjing University of Science and Technology Nanjing 210094 China Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Wuhan 430074 China Engineering Research Center of Functional Polymer Membrane Materials of Jiangsu Province Nanjing Bready Advanced Materials Technology Co. Ltd. Nanjing 211103 China School of Materials Science and Engineering Xiamen University of Technology Xiamen 361024 China

Quasi-two-dimensional perovskite light-emitting diodes (quasi-2D PeLEDs) are emerging as high-potential candidates for new generation of wide-color gamut displays due to their simple, low-cost solution process, and high color purity. However, the luminescence performance of quasi-2D perovskite films is severely limited by dispersed phase distribution and excessive defect density, which are caused by excessive diffusion of nucleation sites during the perovskite growth stage. Here, the benzylphosphonic acid (BPA) molecule, owing to its strong P-O-Pb bond energy sites and strong electronegativity to PEA+, can aggregate lead-halide octahedron to grow high-dimensional phases, avoiding scattered low-dimensional phases (n = 1). The continuous gradient phase distribution will be beneficial to smooth carrier injection and effectively suppress the leakage current in PeLEDs. Meanwhile, the introduction of phosphonic acid groups will fill the vacancies of Pb ions and reduce non-radiative recombination. As a result, the maximum external quantum efficiency (EQE) of PeLEDs can be increased from 8% to 20.6% with a 514 nm light emission and a 21 nm full-width half maximum, and the device lifetime (T 50) is nearly 6-fold of the pristine sample. In addition, this strategy is also suitable for other wavelength. For example, in blue light, performance improvement is also realized that the maximum EQE of 8% and the luminance increased from 1045 to 5264 cd/m2. These results provide a feasible strategy to regulate the phase distribution and passivate the defects of quasi-2D perovskites.

关键词： quasi-2D perovskites light-emitting diodes benzylphosphonic acid phase distribution defect passivation

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MicroRNA-208a silencing against myocardial ischemia/reperfusion injury mediated by reversibly camouflaged biomimetic nanocomplexes

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Nano Research 2023年第8期16卷 11176-11185页

作者： Jianhui Lu Jiaheng Zhang Wen Yan Chenglong Ge Yang Zhou Rongying Zhu Shanzhou Duan Lichen Yin Yongbing Chen Department of Thoracic Surgery Suzhou Key Laboratory of Thoracic OncologyThe Second Affiliated Hospital of Soochow UniversitySuzhou 215004China Center of Stomatology The Second Affiliated Hospital of Soochow UniversitySuzhou 215004China Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Institute of Functional Nano&Soft Materials(FUNSOM)Collaborative Innovation Center of Suzhou Nano Science&TechnologySoochow UniversitySuzhou 215123China

MicroRNA-208a(miR-208a)plays critical roles in the severe fibrosis and heart failure post myocardial ischemia/reperfusion(IR)***-208a inhibitor(mI)with complementary RNA sequence can silence the expression of miR-208a,while it is challenging to achieve efficient and myocardium-targeted ***,biomimetic nanocomplexes(NCs)reversibly coated with red blood cell membrane(RM)were developed for the myocardial delivery of *** construct the NCs,membrane-penetrating helical polypeptide(PG)was first adopted to condense mI and form the cationic inner core,which subsequently adsorbed catalase(CAT)via electrostatic interaction followed by surface coating with *** membrane-coated NCs enabled prolonged blood circulation after systemic administration,and could accumulate in the injured myocardium via passive *** the oxidative microenvironment of injured myocardium,CAT decomposed H_(2)O_(2)to produce O_(2)bubbles,which drove the shedding of the outer RM to expose the positively charged inner core,thus facilitated effective internalization by cardiac *** on the combined contribution of mI-mediated miR-208a silencing and CAT-mediated alleviation of oxidative stress,NCs effectively ameliorated the myocardial microenvironment,hence reducing the infarct size as well as fibrosis and promoting recovery of cardiac *** study provides an effective strategy for the cytosolic delivery of nucleic acid cargoes in the myocardium,and it renders an enlightened approach to resolve the blood circulation/cell internalization dilemma of cell membrane-coated delivery systems.

关键词： myocardial ischemia/reperfusion(IR)injury microRNA-208a silencing red blood cell membrane reversible membrane coating H_(2)O_(2)responsiveness membrane-penetratingα-helical polypeptide

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Ambient Fast Synthesis of Superaerophobic/Superhydrophilic Electrode for Superior Electrocatalytic Water Oxidation

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Energy & Environmental materials 2023年第6期6卷 356-363页

作者： Jingjun Shen Jing Li Bo Li Yun Zheng Xiaozhi Bao Junpo Guo Yan Guo Chenglong Lai Wen Lei Shuangyin Wang Huaiyu Shao Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices Institute of Applied Physics and Materials EngineeringUniversity of MacaoAvenida da UniversidadeTaipaMacaoSAR 999078China Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education Key Laboratory of High Performance Polymer-based Composites of Guangdong ProvinceSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China School of Materials Science and Engineering Huazhong University of Science and TechnologyWuhan 430074China The State Key Laboratory of Refractories and Metallurgy Wuhan University of Science and TechnologyWuhan 430081China State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Developing cost-effective and facile methods to synthesize efficient and stable electrocatalysts for large-scale water splitting is highly desirable but remains a significant *** this study,a facile ambient temperature synthesis of hierarchical nickel-iron(oxy)hydroxides nanosheets on iron foam(FF-FN)with both superhydrophilicity and superaerophobicity is ***,the as-fabricated FF-FN electrode demonstrates extraordinary oxygen evolution reaction(OER)activity with an ultralow overpotential of 195 mV at 10 mA cm^(-2)and a small Tafel slope of 34 mV dec^(-1)in alkaline *** theoretical investigation indicates that the involved lattice oxygen in nickel-iron-based-oxyhydroxide during electrochemical self-reconstruction can significantly reduce the OER reaction overpotential via the dominated lattice oxygen *** rechargeable Zn-air battery assembled by directly using the as-prepared FF-FN as cathode displays remarkable cycling *** is believed that this work affords an economical approach to steer commercial Fe foam into robust electrocatalysts for sustainable energy conversion and storage systems.

关键词： electrocatalysis oxygen evolution reaction oxyhydroxide superaerophobicity superhydrophilicity

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Construction of novel P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt heterophotocathode for enhanced photoelectrochemical water splitting

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Nano Research 2024年第5期17卷 4428-4436页

作者： Jiaru Li Jiayu Bai Songjie Hu Wenyu Yuan Yuyu Bu Xiaohui Guo Key Lab of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education Shaanxi Key Laboratory for Carbon Neutral TechnologyThe College of Chemistry and Materials ScienceNorthwest UniversityXi'an 710069China Key Lab of Wide Band-Gap Semiconductor Materials and Devices School of MicroelectronicsXidian UniversityXi’an 710071China Key Lab of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistryMinistry of EducationSchool of Chemistry&Chemical EngineeringShaanxi Normal UniversityXi'an 710062China

Photoelectrochemical devices have been developed to enable the conversion of solar ***,their commercial potential is restricted by the limited stability of the materials *** enhance the stability of photocathode and its solar water splitting performance,a P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt composite photocathode is developed in this *** novel TiO_(2)/HfO_(2)/MoS_(2) serial nanostructure provides excellent stability of the photocathode,and optimizes the interface energy barrier to further facilitate the transfer process of photogenerated carriers within the *** best P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt photocathode demonstrates an initial potential of 0.5 V(***)and a photocurrent density of-29 mA/cm^(2) at 0 V(***).Through intensity modulated photocurrent spectroscopy and photoluminescence test,it is known that the enhanced water splitting performance is attributed to the optimized carrier transfer *** findings provide a feasible strategy for the stability and photon quantum efficiency enhancement of silicon-based photocathode devices.

关键词： photoelectrochemical water splitting stability surface/interface engineering HfO_(2)layer

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Multiple-resonance thermally activated delayed emitters through multiple peripheral modulation to enable efﬁcient blue OLEDs at high doping levels

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Aggregate 2024年第5期5卷 349-357页

作者： Yuyuan Wang Zhiwei Ma Junrong Pu Danman Guo Gaoyu Li Zhu Chen Shi-Jian Su Huangjun Deng Juan Zhao Zhenguo Chi PCFM Lab GD HPPC LabGuangdong Engineering Technology Research Center for High-Performance Organic and Polymer Photoelectric Functional FilmsState Key Laboratory of Optoelectronic Material and TechnologiesSchool of ChemistrySun Yat-sen UniversityGuangzhouChina State Key Laboratory of Luminescent Materials and Devices and Institute of Polymer Optoelectronic Materials and Devices South China University of TechnologyGuangzhouChina State Key Laboratory of Optoelectronic Material and Technologies School of Materials Science and EngineeringSun Yat-sen UniversityGuangzhouChina

Organic light-emitting diodes(OLEDs)based on multiple resonance-thermallyactivated delayedﬂuorescence(MR-TADF)have the advantages of high excitonutilization and excellent color ***,the large conjugated planarity of gen-eral MR-TADF emitters makes them easily aggregate in the form ofπ–πstacking,resulting in aggregation-caused quenching(ACQ)and the formation of excimers,which reduce exciton utilization efﬁciency and color *** address these issues,large shielding units can be incorporated to prevent interchromophore interactions,whereas the majority of reported molecules are limited to blue-green light *** work proposes a strategy of incorporating steric hindrance groups atdifferent sites of the B/N core to suppress interactions between chromophore,con-tributing to blue MR-TADF emitters with high photo-luminance quantum yields(PLQYs≥95%)and narrow full width at half maximum(FWHM),and importantly,great suppression of the ACQ ***,blue OLEDs achieve high externalquantum efﬁciencies up to 34.3%and high color purity with FWHM of about 27 nmand CIE around(0.12,0.15),even at a high doping concentration of 20 wt%.

关键词： blue emission color purity multiple-resonance organic light-emitting diodes thermally activated delayedﬂuorescence

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An emerging antibacterial nanovaccine for enhanced chemotherapy by selectively eliminating tumor-colonizing bacteria

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Science Bulletin 2024年第16期69卷 2565-2579页

作者： Linfu Chen Zheyu Kang Jingjing Shen Rui Zhao Yu Miao Lin Zhang Zixuan Zheng Zhemin Zhang Nanhui Liu Cheng Wang Huapan Fang Jun Zhou Yudong Wang Zhuang Liu Yang Yang Qian Chen Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Department of Gynecologic Oncology The International Peace Maternity and Child Health HospitalSchool of MedicineShanghai Jiao Tong UniversityShanghai 200030China Department of Thoracic Surgery Shanghai Pulmonary HospitalTongji University School of MedicineShanghai 200433China

Fusobacterium nucleatum(***),an oral anaerobe,is prevalent in colorectal cancer and is closely related to increased cancer cell growth,metastasis,and poor treatment *** vaccines capable of selectively eliminating bacteria present a promising approach to targeting intratumor ***,thereby enhancing cancer *** adjuvants have been employed to enhance the immune response,the vaccine’s effectiveness is constrained by inadequate T-cell activation necessary for eradicating intracellular *** this study,we developed a minimalistic,biomimetic nanovaccine by integrating highly immunostimulatory adjuvant cholesterol-modified CpG oligonucleotides into the autologously derived *** *** to the traditional vaccines consisting of inactivated bacteria and Alum adjuvant,the nanovaccine coupled with bacterial membranes and adjuvants could remarkably improve multiple antigens and adjuvant co-delivery to dendritic cells,maximizing their ability to achieve effective antigen presentation and strong downstream immune ***,the nanovaccine exhibits outstanding selective prophylactic and therapeutic effects,eliminating *** without affecting intratumoral and gut *** significantly enhances chemotherapy efficacy and reduces cancer metastasis in ***-infected colorectal ***,this work represents the rational application of bacterial nanovaccine and provides a blueprint for future development in enhancing the antitumor effect against bacterial-infected cancer.

关键词： Fusobacterium nucleatum Bacterial vaccine Colorectal cancer Biomimetic nanomedicine Chemotherapy

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Constructing lithiophilic sites-rich artificial solid electrolyte interphase to enable dendrite-free and corrosion-free lithium-sulfur batteries

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Green Energy & Environment 2024年第12期9卷 1891-1900页

作者： Wei Lu Anshun Zhao Qiuxu Chen Sihan Liu Mingxi Yu Zihao Wang Ze Gao Xue Zhao Guiru Sun Ming Feng Key Laboratory of Functional Materials Physics and Chemistry Ministry of Education Jilin Normal UniversityChangchunJilin130103China College of Information Technology Jilin Engineering Research Center of Optoelectronic Materials and DevicesJilin Normal UniversitySipingJilin136000China School of Science Changchun University of Science and TechnologyChangchunJilin130022China

An artificial solid electrolyte interphase(SEI)with lithiophilic sites and chemical bonds anchoring lithium polysulfides(LiPSs)has been developed as a potential solution to protect the lithium(Li)metal anode of Lithium-sulfur(Li-S)*** strategy aims to guide consistent Li deposition and relieve lithium ***,the evolution process of lithiophilic sites based on aluminum fluoride(AlF_(3))in an artificial SEI is disclosed in Li-S batteries with metal-based lithiophilic *** polyester polymer(PMMA and PPC)/AlF_(3) artificial SEI(MPAF-SEI)was homogeneously anchored on Li anode by in-situ *** conversion of AlF_(3) into Li-Al and LiF lithiophilic sites effectively reduce the Li nucleation overpotential and prevents the formation of Li *** the same time,the polymer can anchor LiPSs by chemical bonds and prevents Li *** optimized MPAF-SEI protected Li demonstrates excellent stability for over 3000 h at a capacity of 1 mAh cm^(-2) in Li||Li symmetric *** Li-S battery with low N/P(4)exhibits a capacity of 532.6 mAh g^(-1) over 300 cycles lifespan at 0.5 C.

关键词： Li anode SEI Lithiophilic sites Li-S battery AlF_(3)

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Modulating surface oxygen species via facet engineering for efficient conversion of nitrate to ammonia

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Journal of Energy Chemistry 2023年第3期78卷 211-221,I0007页

作者： Wenye Zhong Zhiheng Gong Zuyun He Nian Zhang Xiongwu Kang Xianwen Mao Yan Chen School of Environment and Energy State Key Laboratory of Pulp and Paper EngineeringSouth China University of TechnologyGuangzhou 510006GuangdongChina State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China Department of Materials Science and Engineering National University of SingaporeSingapore 119077Singapore Institute of Functional Intelligent Materials National University of SingaporeSingapore 119077Singapore Centre for Advanced 2D Materials National University of SingaporeSingapore 119077Singapore

Electrochemical reduction of nitrate,a common pollutant in aquatic environment,to valuable ammonia(NO3-RR) using renewably-sourced electricity has attracted widespread interests,with past efforts mainly focused on designing electrocatalysts with high activity and *** detailed correlation between catalyst properties and NO3-RR kinetics,nevertheless,is still not fully *** this work,we modulate the surface oxygen species of Cu_(2)O via facet engineering,and systematically study the impact of these oxygen species on the NO_(3)^(-)RR *** advanced spectroscopic techniques,densi ty fu n ctional theory calculations and molecular dynamics simulations,we find that while oxygen vacancies on Cu_(2)O(111) surface promote the adsorption of reactants and reaction intermediates,hydroxyl groups effectively inhibit the side reaction of hydrogen evolution and facilitate the hydrogenation process of *** two effects work in concert to render Cu_(2)O(111) facet the highest NO3-RR activity relative to those from other *** study provides critical insights into the synergistic effect of exposed facets and surface oxygen species on heterogeneous catalysis,and offers a generalizable,facet engineeringbased strategy for improving the performance of a variety of electrocatalysts important for renewable energy conversion.

关键词： Facet engineering Oxygen vacancy Hydroxyl group Electrochemical nitrate reduction Ammonia

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