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Nano Research 2024年第9期17卷 8134-8144页

作者： Jihao Su Ling Yang Dengbin Yu Shaojun Dong State key laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China College of chemistry Jilin UniversityChangchun 130022China University of Science and Technology of China Hefei 230026China

A significant challenge in developing high-performance hybrid supercapacitors(HSCs)is the need to reasonably construct advanced architectures that consist of various components and exhibit superior electrochemical capacitance *** FeCoNi-layered double hydroxide(FeCoNi-LDH)porous material has a specific capacitance of 1960 F·g^(-1)when used as the anode material at 1 A·g^(-1).The FeCoNi-LDH material exhibits nanoplates with a distinct spindle morphology on their *** to the combined action of the three metals and abundant oxygen vacancies,they exhibit unique rate performance and cycle *** electronic structure of LDH and the regulation of oxygen vacancy were confirmed by density functional theory(DFT)*** suggests that the strength of hydroxide can reduce the energy required for oxygen vacancy formation in FeCoNi-LDH nanosheets and enhance ion and charge transfer,as well as electrolyte adsorption on the electrode *** FeCoNi-LDH//activated carbon(AC)HSC has an energy density of 53.2 Wh·kg^(-1)at a power density of 800 W·kg^(-1),surpassing other devices composed of comparable materials during the same *** study made significant advances in the design and synthesis of a ternary LDH porous structure with distinct oxygen vacancies,as well as its potential application in electrochemical energy storage.

关键词： oxygen vacancy FeCoNi-layered double hydroxide(FeCoNi-LDH) theory calculation electrode material hybrid supercapacitor

Regulating Signal Pathway Triggers Circular Reactive Oxygen Species Production to Augment Oxidative Stress with Enzyme-Activated Nanoparticles

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CCS chemistry 2024年第3期6卷 693-708页

作者： Benkai Bao Qiong Yuan Qian Feng Ling Li Meiqi Li Yanli Tang key laboratory of Analytical chemistry for Life Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistryMinistry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’anShaanxi Province 710119

Regulating antioxidative stress pathways to augment oxidative stress and enhance antitumor therapy is highly desirable but very ***,we initiated a multifunctional nanoparticle to regulate the Keap1-Nrf2 antioxidative stress pathway to promote cancer cell *** OPFV-SnMP@GE11 nanoparticles were assembled by enzyme-activated OPFV-TLQ,tin mesoporphyrin(SnMP),and ***-SnMP@GE11 accumulated at tumor sites through specific targeting with ***-TLQ was specifically reduced to a photosensitizer OPFVNH2 by endocellular NAD(P)H:quinone oxidoreductase 1(NQO1).Under irradiation,OPFV-NH2 greatly produced reactive oxygen species(ROS)through a type I mechanism,which activated the Keap1-Nrf2 signal pathway and enhanced the transcription of NQO1,resulting in a continuous and explosive generation of ***,SnMP inhibited the activity of heme oxygenase-1(HO-1),further depressing antioxidative *** strategy provides insight into the regulation of the signal pathway to amplify oxidative stress,paving the way to studying the molecular mechanisms of cellular activities to enhance cancer therapy.

关键词： Keap1-Nrf2 pathway enzyme-activated probe reactive oxygen species oxidative stress antitumor therapy

Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li Department of chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State key laboratory of Surface Physics and Department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable ***,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as *** key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon *** mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion *** method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

Engineering oxygen vacancies on Tb-doped ceria supported Pt catalyst for hydrogen production through steam reforming of long-chain hydrocarbon fuels

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Chinese Journal of Chemical Engineering 2024年第4期68卷 181-192页

作者： Zhourong Xiao Changxuan Zhang Peng Li Desong Wang Xiangwen Zhang Li Wang Jijun Zou Guozhu Li State key laboratory of Metastable Materials Science and Technology(MMST) Hebei Key Laboratory of Applied ChemistryCollege of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004China key laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell *** this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation *** physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron *** results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported *** catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was *** with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min.

关键词： Steam reforming n-Dodecane Hydrogen production Pt-based catalyst Oxygen vacancy CeO_(2)

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Highly selective adsorption of rhenium by amyloid-like protein material

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Science China(Technological Sciences) 2024年第5期67卷 1417-1430页

作者： MUHAMMAD Arif YANG QingMin KANWAL Aisha ZHAO Jian NAWAZ Mohsan REN Hao YANG Peng key laboratory of applied Surface and Colloid chemistry Ministry of Education Xi’an key laboratory of Polymeric Soft Matter International Joint Research Center on Functional Fiber and Soft Smart TextileSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an710119China School of chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an710072China

Rhenium separation from molybdenum in molybdenite minerals and waste leachate has become an emerging *** this challenge,we prepared a set of protein-based alkylamine/alkylammonium salts complexes as extractants for selective uptake of rhenium from molybdenum,where the protein component turned into the insoluble amyloid-like structure when its internal disulfide bonds were reduced,namely phase-transition *** them,the phase-transited lysozyme and methyletrioctyleammonium chloride complex(PTL-N263)exhibited the most efficient adsorption at the alkaline condition for the electrostatic interaction between negatively charged metal ions with positively charged center(R_(4)N^(+))in N263,where negatively charged protein residues hindered the ion exchange of Cl^(-)in N263 for larger size Mo species(Mo_(7)O_(24)^(6-))than smaller size Re species(ReO^(4-)).The adsorption follows the Freundlich model and pseudo-second-order kinetics,which exhibits toplevel adsorption performance with a maximum adsorption capacity of 124 mg/g and a separation factor(β_(Re/Mo))of 2.78×10^(3)for *** adsorption capacity per unit area(57.2 mg/(g m^(2)))is 1.6–41 times higher than previously reported adsorbents,and the cost for adsorbing 1 g of Re(VII)is$1.07,indicating its industrial *** adsorption strategy can be applied to separating Re from Mo in binary solutions and industrial wastewater with other competing ions.

关键词： amyloid phase-transited lysozyme selective adsorption rhenium waste leachate solution

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Sequential enantioselective Ugi-4CR/post-Ugi transformation strategy:a precise construction of structurally diverse azaspiro polycyclic scaffolds

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Science China chemistry 2024年第2期67卷 576-586页

作者： Xiao-Bao Wu Jun-Xiu Shi Yi-Ming Ou Hua-Jie Jiang Yi-Jun Fang Qi-Ming Wang Quan Gao Jie Yu Department of applied chemistry Anhui Province Engineering Laboratory for Green Pesticide Development and ApplicationAnhui Province Key Laboratory of Crop Integrated Pest ManagementAnhui Agricultural UniversityHefei230036China

A privileged strategy has been developed for the precise construction of enantioenriched azaspiro polycyclic *** diverse azaspiro polycycles bearing multiple contiguous stereocenters are obtained with excellent results(up to 99:1 e.r.,>95:5 d.r.) via sequential enantioselective four-component Ugi reactions/post-Ugi transformations with substrates containing prerequisite functional groups in the presence of anionic stereogenic-at-cobalt(Ⅲ) complexes.

关键词： asymmetric catalysis post-Ugi transformation anionic stereogenic-at-cobalt(Ⅲ)complex azaspiro polycyclic scaffold one-pot synthesis

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Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction

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Carbon Energy 2024年第3期6卷 276-286页

作者： Tingyi Zhou Yi Guan Changjie He Lei Zhang Xueliang Sun Zhongxin Song Qianling Zhang Chuanxin He Xiantao Jiang Zhaoyan Luo Wei Xing Xiangzhong Ren College of chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina Department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada State key laboratory of Electroanalytical chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesJilinChangchunChina

The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to ***,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C ***,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation *** found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe *** as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,***,the catalyst also represents excellent durability exceeding that of Fe–N–C SA *** practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery *** work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.

关键词： d-band center metal clusters oxygen reduction reaction single-atom catalyst site occupations strategy

Synergistic enhancement of ultrasound therapy for tumors using hypoxia-activated 6-diazo-5-oxo-L-norleucine(DON)prodrug nanoparticles

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Nano Research 2024年第7期17卷 6323-6331页

作者： Mengfei Zheng Zhilin Liu Hang Xu Daping Ye Linjie Cui Chenguang Yang Lili Ma Kun Wang Kazuo Sakurai Zhaohui Tang key laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Jilin Biomedical Polymers Engineering laboratory Changchun 130022China Department of chemistry and Biochemistry The University of Kitakyushu1-1 HibikinoKitakyushu 808-0135Japan

Ultrasound(US)has been applied in clinical practice for its non-invasive and high ***,it is difficult to achieve a satisfactory anti-tumor effect with US ***,the use of US therapy alone can exacerbate tumor *** this study,we prepared hypoxia-activated 6-diazo-5-oxo-L-norleucine(DON)prodrug nanoparticles(HDON-NPs)to improve US therapeutic *** an H22 murine liver cancer model,US therapy selectively disrupted tumor blood vessels,leading to increased tumor hypoxia and a 1.67-fold increase in the expression of nitroreductase(NTR).The combination therapy of US and HDON-NPs demonstrated a synergistic effect,resulting in a tumor suppression rate(TSR)of 90.2%±6.4%,which was 5.93-fold higher than that of US therapy *** combined treatment selectively blocked the glutamine metabolism of the tumor cells while simultaneously activating the T cells in the tumor microenvironment,thereby exerting a robust anti-tumor effect.

关键词： ultrasound therapy hypoxia-activated prodrug nanoparticles 6-diazo-5-oxo-L-norleucine(DON) glutamine antagonist starvation therapy

High-speed flexible near-infrared organic photodiode for optical communication

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National Science Review 2024年第3期11卷 227-238页

作者： Yu Zhu Hongbin Chen Ruiman Han Hao Qin Zhaoyang Yao Hang Liu Yanfeng Ma Xiangjian Wan Guanghui Li Yongsheng Chen The Centre of Nanoscale Science and Technology and key laboratory of Functional Polymer Materials Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer Materials College of Chemistry and Renewable Energy Conversion and Storage Center(RECAST) Nankai University State key laboratory of Elemento-Organic chemistry Nankai University

Optical communication is a particularly compelling technology for tackling the speed and capacity bottlenecks in data communication in modern society. Currently, the silicon photodetector plays a dominant role in high-speed optical communication across the visible-near-infrared spectrum. However, its intrinsic rigid structure, high working bias and low responsivity essentially limit its application in next-generation flexible optoelectronic devices. Herein, we report a narrow-bandgap non-fullerene acceptor（NFA） with a remarkable π-extension in the direction of both central and end units（CH17） with respect to the Y6 series, which demonstrates a more effective and compact 3D molecular packing, leading to lower trap states and energetic disorders in the photoactive film. Consequently, the optimized solution-processed organic photodetector（OPD） with CH17 exhibits a remarkable response time of 91 ns（λ = 880 nm） due to the high charge mobility and low parasitic capacitance, exceeding the values of most commercial Si photodiodes and all NFA-based OPDs operating in self-powered mode. More significantly, the flexible OPD exhibits negligible performance attenuation（<1%） after bending for 500 cycles, and maintains 96% of its initial performance even after 550 h of indoor exposure. Furthermore, the high-speed OPD demonstrates a high data transmission rate of 80 MHz with a bit error rate of 3.5 × 10-4, meaning it has great potential in next-generation high-speed flexible optical communication systems.

关键词： flexible organic photodetector high-speed NIR organic photodetector optical communication light fidelity narrow-bandgap non-fullerene acceptors

Manipulating fast Li_(2)S redox via carbon confinement and oxygen defect engineering of In_(2)O_(3)for lithium-sulfur batteries

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Nano Research 2024年第6期17卷 5179-5187页

作者： Jinlei Qin Rui Wang Zilong Yuan Pei Xiao Deli Wang key laboratory of Material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Lithium-sulfur(Li-S)batteries have been considered as promising energy storage systems due to the merits of high energy density and low ***,the lithium polysulfides(LiPSs)diffusion and sluggish redox kinetics hamper t... 详细信息

关键词： Li-S batteries nitrogen-doped carbon confinement oxygen vacancies bidirectional Li_(2)S redox