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Dual-conductive metal-organic framework@MXene heterogeneity stabilizes lithium-ion storage

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Journal of Energy Chemistry 2023年第1期76卷 368-376,I0009页

作者： Lanju Sun Honglei Wang Shengliang Zhai Jikai Sun Xu Fang Hongyan Yang Dong Zhai Chengcheng Liu Wei-Qiao Deng Hao Wu institute of molecular Sciences and engineering Institute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao 266237ShandongChina

Although a few pristine metal-organic frameworks(MOFs) of graphene analogue topology exhibit high intrinsic electrical conductivity, their use in lithium-ion batteries(LIBs) is still hampered by unfavorable Li+adsorption energy(ΔEa). In this paper, an electroconductive ferrocene-based MOF@MXene heterostructure is built to provide stable anodes for Li+storage. Charge density difference and planar average potential charge density show substantial redistribution of charges at the interfaces, transferring from MXene to MOF layers. Moreover, density functional theory(DFT) calculations reveal that the interaction between MXene and MOF significantly increases the ΔEa. As a result, the heterostructure anode exhibits high capacities and outstanding cycling stability with a capacity retention of 80% after 5000 cycles at 5 A g^(-1), outperforming mono-component MXene and MOF. Furthermore, the heterostructure anode is built into a full cell with a commercial NCM 532 cathode, delivering a high energy density of 611 Wh kg^(-1)and power density of 7600 W kg^(-1). The developed conductive MOF@MXene heterogeneity for improved LIB offers valuable insights into the design of advanced electrode materials for energy storage.

关键词： MXene Metal-organic framework Heterostructure Lithium-ion battery Adsorption energy

Atomically Substitutional engineering of Transition Metal Dichalcogenide Layers for Enhancing Tailored Properties and Superior Applications

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Nano-Micro Letters 2024年第5期16卷 248-284页

作者： Zhaosu Liu Si Yin Tee Guijian Guan Ming‑Yong Han institute of molecular Plus Tianjin UniversityTianjin 300072People’s Republic of China institute of Materials Research and engineering A*STARSingapore 138634Singapore

Transition metal dichalcogenides(TMDs)are a promising class of layered materials in the post-graphene era,with extensive research attention due to their diverse alternative elements and fascinating semiconductor behavior.Binary MX2 layers with different metal and/or chalcogen elements have similar structural parameters but varied optoelectronic properties,providing opportunities for atomically substitutional engineering via partial alteration of metal or/and chalcogenide atoms to produce ternary or quaternary TMDs.The resulting multinary TMD layers still maintain structural integrity and homogeneity while achieving tunable(opto)electronic properties across a full range of composition with arbitrary ratios of introduced metal or chalcogen to original counterparts(0–100%).Atomic substitution in TMD layers offers new adjustable degrees of freedom for tailoring crystal phase,band alignment/structure,carrier density,and surface reactive activity,enabling novel and promising applications.This review comprehensively elaborates on atomically substitutional engineering in TMD layers,including theoretical foundations,synthetic strategies,tailored properties,and superior applications.The emerging type of ternary TMDs,Janus TMDs,is presented specifically to highlight their typical compounds,fabrication methods,and potential applications.Finally,opportunities and challenges for further development of multinary TMDs are envisioned to expedite the evolution of this pivotal field.

关键词： Transition metal dichalcogenides Atomic substitution Tailored structure Tunable bandgap Enhanced applications

Heteroatom doping regulates the catalytic performance of singleatom catalyst supported on graphene for ORR

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Nano Research 2024年第3期17卷 1086-1093页

作者： Ji-Kai Sun Yu-Wei Pan Meng-Qian Xu Lei Sun Shaolong Zhang Wei-Qiao Deng Dong Zhai institute of molecular Sciences and engineering Institute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao 266237China College of Chemistry and Environmental engineering Shenzhen UniversityShenzhen 518060China

Replacing fossil fuels with fuel cells is a feasible way to reduce global energy shortages and environmental pollution.However,the oxygen reduction reaction(ORR)at the cathode has sluggish kinetics,which limits the development of fuel cells.It is significant to develop catalysts with high catalytic activity of ORR.The single-atom catalysts(SACs)of Pt supported on heteroatom-doped graphene are potential candidates for ORR.Here we studied the SACs of Pt with different heteroatoms doping and screened out Pt-C_(4) and Pt-C_(3)O_(1) structures with only 0.13 V overpotential for ORR.Meanwhile,it is found that B atoms doping could weaken the adsorption capacity of Pt,while N or O atoms doping could enhance it.This regularity was verified on Fe SACs.Through the electronic interaction analysis between Pt and adsorbate,we explained the mechanism of this regularity and further proposed a new descriptor named corrected d-band center(ε_(d-corr))to describe it.This descriptor is an appropriate reflection of the number of free electrons of the SACs,which could evaluate its adsorption capacity.Our work provides a purposeful regulatory strategy for the design of ORR catalysts.

关键词： single-atom catalyst(SAC) oxygen reduction reaction(ORR) heteroatom doping corrected d-band center descriptor

Monitoring the in vivo siRNA release from lipid nanoparticles based on the fluorescence resonance energy transfer principle

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Asian Journal of Pharmaceutical Sciences 2023年第1期18卷 72-85页

作者： Lei Sun Jinfang Zhang Jing-e Zhou JingWang Zhehao Wang Shenggen Luo Yeying Wang Shulei Zhu Fan Yang Jie Tang Wei Lu Yiting Wang Lei Yu Zhiqiang Yan institute of Biomedical engineering and Technology Shanghai Engineering Research Center of Molecular Therapeutics and New Drug DevelopmentSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China Shanghai engineering Research Center of molecular Therapeutics and New Drug Development School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China

The siRNA-loaded lipid nanoparticles have attracted much attention due to its significant gene silencing effect and successful marketization.However,the in vivo distribution and release of siRNA still cannot be effectively monitored.In this study,based on the fluorescence resonance energy transfer(FRET)principle,a fluorescence dye Cy5-modified survivin siRNA was conjugated to nanogolds(Au-DR-siRNA),which were then wrapped with lipid nanoparticles(LNPs)for monitoring the release behaviour of siRNA in vivo.The results showed that once Au-DR-siRNA was released from the LNPs and cleaved by the Dicer enzyme to produce free siRNA in cells,the fluorescence of Cy5 would change from quenched state to activated state,showing the location and time of siRNA release.Besides,the LNPs showed a significant antitumor effect by silencing the survivin gene and a CT imaging function superior to iohexol by nanogolds.Therefore,this work provided not only an effective method for monitoring the pharmacokinetic behaviour of LNP-based siRNA,but also a siRNA delivery system for treating and diagnosing tumors.

关键词： Survivin siRNA Lipid nanoparticles In vivo release Nanogolds Fluorescence resonance energy transfer

Chemical characteristics and source apportionment of PM_(2.5) between heavily polluted days and other days in Zhengzhou, China

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Journal of Environmental Sciences 2018年第4期30卷 188-198页

作者： Nan Jiang Qiang Li Fangcheng Su Qun Wang Xue Yu Panru Kang Ruiqin Zhang Xiaoyan Tang Research institute of Environmental Science College of Chemistry and Molecular Engineering Zhengzhou University

PM（2.5） samples were collected in Zhengzhou during 3 years of observation, and chemical characteristics and source contribution were analyzed. Approximately 96% of the daily PM（2.5） concentrations and annual average values exceeded the Chinese National Ambient Air Quality Daily and Annual Standards, indicating serious PM（2.5） pollution. The average concentration of water-soluble inorganic ions was 2.4 times higher in heavily polluted days（daily PM32.5 concentrations ＆gt; 250 μg/mand visibility ＆lt; 3 km） than that in other days, with sulfate, nitrate, and ammonium as major ions. According to the ratio of NO-3/SO2-4,stationary sources are still the dominant source of PM（2.5） and vehicle emission could not be ignored. The ratio of secondary organic carbon to organic carbon indicated that photochemical reactivity in heavily polluted days was more intense than in other days.Crustal elements were the most abundant elements, accounting for more than 60% of 23 elements. Chemical Mass Balance results indicated that the contributions of major sources（i.e., nitrate, sulfate, biomass, carbon and refractory material, coal combustion, soil dust,vehicle, and industry） of PM（2.5） were 13%, 16%, 12%, 2%, 14%, 8%, 7%, and 8% in heavily polluted days and 20%, 18%, 9%, 2%, 27%, 14%, 15%, and 9% in other days, respectively.Extensive combustion activities were the main sources of polycyclic aromatic hydrocarbons during the episode（Jan 1-9, 2015） and the total benzo[a]pyrene equivalency concentrations in heavily polluted days present significant health threat. Because of the effect of regional transport, the pollution level of PM（2.5） in the study area was aggravated.

关键词： PM2.5 Water soluble inorganic ions Secondary organic carbon CMB Back trajectory analysis

Light-induced stepped thermal relaxation in a Hofmann-type metal-organic framework

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Science China Chemistry 2024年第6期67卷 1983-1989页

作者： Wen Cui Wei-Wei Wu Ze-Yu Ruan Yan-Cong Chen Guang-Jun Zeng Guan-Xi Chen Si-Guo Wu Zhao-Ping Ni Ming-Liang Tong Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education School of ChemistryInstitute of Green Chemistry and Molecular EngineeringGuangdong Basic Research Center of Excellence for Functional Molecular EngineeringSun Yat-sen UniversityGuangzhou510275China

Spin-crossover(SCO)materials with light-induced multistability have potential applications in multi-addressable opto-magnetic memory devices and multiple switches.Here,we reported a three-dimensional Hofmann-type metal-organic framework(MOF)[Fe(bpy){Pt(CN)_(4)}]·coumarin(1·coumarin,bpy=4,4′-bipyridine),which exhibits an incomplete and hysteretic SCO behavior.Most importantly,the light-induced stepped thermal relaxation(LISTR)with obvious magnetic plateau for a hidden intermediate spin state is firstly realized.This hidden spin state is also observed for the first time in the thermal relaxation after light-assisted spin state annealing(LASSA).Meanwhile,an extremely rare bi-directional light-induced excited spin-state trapping(LIESST)with the highest reverse-LIESST temperature is observed.Therefore,five spin states can be captured in 1·coumarin and the tristability can be modulated below 102 K through the excitation-relaxation mechanism.Hence,the light-and temperatureinduced multistability provides a new strategy for developing multistable materials.

关键词： light magnetic multistability iron metal-organic framework spin-crossover

Regulation of excitation energy transfer in Sb-alloyed Cs_(4)MnBi_(2)Cl_(12) perovskites for efficient CO_(2) photoreduction to CO and water oxidation toward H_(2)O_(2)

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Journal of Energy Chemistry 2023年第7期82卷 18-24,I0001页

作者： Haiwen Wei Zhen Li Honglei Wang Yang Yang Pengfei Cheng Peigeng Han Ruiling Zhang Feng Liu Panwang Zhou Keli Han institute of molecular Sciences and engineering Institute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao 266237ShandongChina State Key Laboratory of molecular Reaction Dynamics Dalian Institute of Chemical PhysicsChinese Academy of ScienceDalian 116023LiaoningChina

Lead(Pb)-free halide perovskites have recently attracted increasing attention as potential catalysts for CO_(2) photoreduction to CO due to their potential to capture solar energy and drive catalytic reaction.However,issues of the poor charge transfer still remain one of the main obstacles limiting their performance due to the overwhelming radiative and nonradiative charge-carrier recombination losses.Herein,Pb-free Sb-alloyed all-inorganic quadruple perovskite Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12)(0≤x≤1)is synthesized as efficient photocatalyst.By Sb alloying,the undesired relaxation of photogenerated electrons from conduction band to emission centers of[MnCl6]^(4-)is greatly suppressed,resulting in a weakened PL emission and enhanced charge transfer for photocatalyst.The ensuing Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12) photocatalyst accomplishes efficient conversion of CO_(2)into CO,accompanied by a surprising production of H_(2)O_(2),a high valueadded product associated with water oxidation.By optimizing Sb^(3+) concentration,a high CO evolution rate of 35.1μmol g^(-1)h^(-1)is achieved,superior to most other Pb and Pb-free halide perovskites.Our findings provide new insights into the mixed-cation alloying strategies for improved photocatalytic performance of Pb-free perovskites and shed light on the rational design of robust band structure toward efficient energy transfer.

关键词： Pb-free perovskites Energy band modulation Perovskite photocatalysis photocatalytic CO_(2)reduction Water oxidation to H_(2)O_(2)

Polycarcin V induces DNA-damage response and enables the profiling of DNA-binding proteins

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National Science Review 2022年第11期9卷 19-28页

作者： Zongwei Yue Fan Wu Fusheng Guo Jiyeong Park Jin Wang Liyun Zhang Daohong Liao Wenyang Li Orlando D.Sch?rer Xiaoguang Lei Beijing National Laboratory for molecular Sciences Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationDepartment of Chemical BiologyCollege of Chemistry and Molecular Engineering Synthetic and Functional Biomolecules CenterPeking University Peking-Tsinghua Center for Life Science Academy for Advanced Interdisciplinary Studies Peking University Center for Genomic Integrity Institute for Basic Science Jiangsu JITRI molecular engineering Inst.Co. Ltd. Department of Biological Sciences School of Life Sciences Ulsan National Institute of Science and Technology institute for Cancer Research Shenzhen Bay Laboratory

To maintain genomic integrity and avoid diseases, the DNA-damage response(DDR) not only detects and repairs DNA lesions, but also contributes to the resistance to DNA-damaging chemotherapeutics.Targeting the DDR plays a significant role in drug discovery using the principle of synthetic lethality. The incomplete current knowledge of the DDR encouraged us to develop new strategies to identify and study its components and pathways. Polycarcin V, belonging to the C-aryl glycoside natural products, is a light-activatable DNA-intercalating agent that causes DNA damage by forming a covalent [2+2]cycloadduct with thymine residue under 365–450 nm of light irradiation in a DNA-sequence-independent manner. Taking advantage of the light-activatable feature and temporal control of DDR, we designed and synthesized polycarcin V-based bifunctional chemical probes, including one that cross-links DNA to DNA-binding protein to explore the DDR induced by polycarcin V and uncover novel DNA–protein interactions. Utilizing this chemical probe and activity-based protein profiling-stable isotope labeling with amino acids in cell culture, we identified 311 DNA-binding protein candidates, including known DDR factors and additional proteins that may be of interest in discovering new biology. We validated our approach by showing that our probe could specifically cross-link proteins involved in nucleotide excision repair(NER) that repair bulky DNA adducts. Our studies showed that the [2+2] cycloadduct formed by polycarcin V could indeed be repaired by NER in vivo. As a DNA-damaging agent, polycarcin V or its drug-like derivative plus blue light showed promising properties for psoriasis treatment, suggesting that it may itself hold promise for clinic applications.

关键词： polycarcin V [2+2] DNA photoadduct light-activatable chemical probe ABPP for DNA-binding protein proteomics psoriasis treatment

Rational design of a turn-on fluorescent probe for visualization of GRP78 protein in tumor models

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Chinese Chemical Letters 2023年第3期34卷 352-355页

作者： Ying Wen Ning Jing Fangjun Huo Caixia Yin institute of molecular Science Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of EducationShanxi UniversityTaiyuan 030006China Research institute of Applied Chemistry Shanxi UniversityTaiyuan 030006China

Fluorescence image for accurate tumor label still faces challenges in cancer detection and diagnostics.Emerging evidence is indicating that glucose-regulated protein 78(GRP78), a stress-inducible protein chaperone, is a great potential biomarker and therapeutic target for cancer. However, currently available probe for image tumor based on GRP78 has not been reported, owning to no obvious strategy in probe design towards this protein. In this paper, a hairpin-shaped peptidyl probe(pep FAM) conjugated with a 5-FAM fluorophore and a dabcyl quencher at both ends was developed, respectively. The probe was designed by performing a traditional fluorescence resonance energy transfer mechanism and employing a GRP78 specifically-binding peptide. Furthermore, the probe was used to specifically image cancer cells,and accurately image xenograft tumors in mice models. The novel fluorescent probe is expected to be a useful tool for the diagnostics of cancer.

关键词： Glucose-regulated protein 78 Fluorescence probe Living cell imaing Tumor diagnosis