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Approaches to Improving Selectivity During Photoelectrochemical Transformation of Small Molecules

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Transactions of Tianjin University 2024年第2期30卷 167-177页

作者： Sipeng Yang Jie Yang Mengyu Duan Shirong Kang Shaohua He Chuncheng Chen Key Laboratory of Photochemistry CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100190China

Photoelectrochemical (PEC) small-molecule oxidation can selectively transform substrates into high-value-added fine chemicals and increase the rate of cathode hydrogen evolution. Nevertheless, achieving high-selectivity PEC oxidation of small molecules to produce specific products is a very challenging task. In general, selectivity can be improved by changing the surface catalyticsites of the photoanode and modulating the interfacial environments of the reactions. Herein, recent advances in approaches to improving selective PEC oxidation of small molecules are introduced. We first briefly discuss the basic concept and fundamentals of small-molecule PEC oxidation. The reported approaches to improving the performance of selective PEC oxidation of small molecules are highlighted from two aspects: (1) changing the surface properties of photoanodes by selecting suitable materials or modifying the photoanodes and (2) mediating the oxidation reactions using redox mediators. The PEC oxidation mechanism of these studies is emphasized. We also discuss the challenges in this research direction and offer a perspective on the further development of selective PEC-based small-molecule transformation.

关键词： Photoelectrocatalytic Small-molecule oxidation Improving selectivity Surface properties Mediating

Bunching enhancement for coherent harmonic generation by using phase merging effects

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Matter and Radiation at Extremes 2024年第5期9卷 10-21页

作者： Ke Feng Kangnan Jiang Runshu Hu Shixia Luan Wentao Wang Ruxin Li State Key Laboratory of High Field Laser Physics and CAS center for excellence in Ultra-intense Laser Science Shanghai Institute of Optics and Fine Mechanics(SIOM)Chinese Academy of Sciences(CAS)ShanghaiPeople’s Republic of China School of Physical Science and Technology ShanghaiTech UniversityShanghaiPeople’s Republic of China center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijingPeople’s Republic of China

In this paper,promising but simple schemes are investigated to enhance the micro-bunching of relativistic electron beams for coherent harmonic generation(CHG)by using phase merging *** contrast to the standard CHG scheme,two specially designed dispersion sections(DSs)are adopted with the DS-modulator–DS *** phase space of the e beam is appropriately coupled in the first DS,and the electrons within one seed wavelength can merge to the same phase with a matched second ***-bunching of the e beam can thus be enhanced by a large margin with much higher-harmonic *** e beams from laser wakefield accelerators(LWFAs)as an example,start-to-end simulations are performed to show the effectiveness and robustness of the proposed schemes with several *** beam current can be optimized to several tens to hundreds of kiloamperes,and the radiation power reaches hundreds of megawatts in the extreme ultraviolet regime within a 3.5 m-long *** proposed schemes offer new opportunities for future compact free-electron lasers driven by LWFAs and provides prospects for truly compact and widely applicable systems.

关键词： modulator harmonic phase

Unlocking supercapacitive energy storage potential:Catalyzing electrochemically inactive manganese oxides to active MnO_(2)via heterostructure reconstruction

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Nano Research 2024年第7期17卷 5897-5906页

作者： Baohong Zhang Tao Jiang Xinyan Zhou Xiaoyu Fan Binbin Jia Lidong Li School of Chemistry Beihang UniversityBeijing 100191China College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChinaThree Gorges UniversityYichang 443002China Chinese Academy of Sciences(CAS)Key Laboratory of Nanosystem and Hierarchy Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China Shanghai GTX Semiconductor Co. Ltd.Shanghai 201806China

Advancing supercapacitor system performance hinges on the innovation of novel electrode materials seamlessly integrated within distinct ***,we introduce a direct approach for crafting nanorod arrays featuring crystalline/amorphous CuO/MnO_(2)−*** reconfigured heterostructure results in an elevated content of electrochemically active MnO_(2).The nanorod arrays serve as efficient capacitive anodes and are easily prepared via low-potential electrochemical *** resulting structure spontaneously forms a p–n heterojunction,developing a built-in electric field that dramatically facilitates the charge transport *** intrinsic electric field,in conjunction with the crystalline/amorphous architecture,enables a large capacitance of 1.0 F·cm^(−2)at 1.0 mA·cm^(−2),an ultrahigh rate capability of approximately 85.4%at 15 mA·cm^(−2),and stable cycling performance with 92.4%retention after 10,000 *** calculations reveal that the presence of heterojunctions allows for the optimization of the electronic structure of this composite,leading to improved conductivity and optimized OH−adsorption *** work provides new insights into the rational design of heterogeneous nanostructures,which hold great potential in energy storage applications.

关键词： reconfiguration active MnO_(2) crystalline/amorphous structure p-n heterojunction supercapacitor

Recent advances in bioinspired vision systems with curved imaging structures

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Rare Metals 2024年第4期43卷 1407-1434页

作者： Ze-Ping He Xun Han Wen-Qiang Wu Zhang-Sheng Xu Cao-Feng Pan CAS center for excellence in Nanoscience Beijing Key Laboratory of Micro-Nano Energy and SensorBeijing Institute of Nanoenergy and NanosystemsChinese Academy of SciencesBeijing100083China School of Nanoscience and Technology University of Chinese Academy of SciencesBeijing100049China ZJU-Hangzhou Global Scientific and Technological Innovation center School of Micro-Nano ElectronicsZhejiang UniversityHangzhou311200China Institute of Microscale Optoelectronics Shenzhen UniversityShenzhen518060China

Limited by the planar imaging structure,the commercial camera needs to introduce additional optical elements to compensate for the curved focal plane to match the planar image *** results in a complex and bulky *** contrast,biological eyes possess a simple and compact structure due to their curved imaging structure that can directly match with the curved focal *** by the structures and functions of biological eyes,curved vision systems not only improve the image quality,but also offer a variety of advanced ***,we review the recent advances in bioinspired vision systems with curved imaging ***,we focus on their applications in implementing different functions of biological eyes,as well as the emerging curved neuromorphic imaging systems that incorporate bioinspired optical and neuromorphic processing *** addition,the challenges and opportunities of bioinspired curved imaging systems are also discussed.

关键词： Bioinspired Curved vision system Compound eye Chambered eye Neuromorphic

Vector magnetometry in zero bias magnetic field using nitrogen-vacancy ensembles

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Chinese Physics B 2024年第10期33卷 21-29页

作者： Chunxing Li Fa-Zhan Shi Jingwei Zhou Peng-Fei Wang CAS Key Laboratory of Microscale Magnetic Resonance and School of Physical Sciences University of Science and Technology of ChinaHefei 230026China CAS center for excellence in Quantum Information and Quantum Physics University of Science and Technology of ChinaHefei 230026China Hefei National Laboratory University of Science and Technology of ChinaHefei 230088China

The application of the vector magnetometry based on nitrogen-vacancy(NV)ensembles has been widely investigatedin multiple *** has the superiority of high sensitivity and high stability in ambient conditions with microscale ***,a bias magnetic field is necessary to fully separate the resonance lines of optically detected magneticresonance(ODMR)spectrum of NV *** brings disturbances in samples being detected and limits the rangeof ***,we demonstrate a method of vector magnetometry in zero bias magnetic field using NV *** utilizing the anisotropy property of fluorescence excited from NV centers,we analyzed the ODMR spectrum of NVensembles under various polarized angles of excitation laser in zero bias magnetic field with a quantitative numerical modeland reconstructed the magnetic field *** minimum magnetic field modulus that can be resolved accurately is downto~0.64 G theoretically depending on the ODMR spectral line width(1.8 MHz),and~2 G experimentally due to noisesin fluorescence signals and errors in *** using 13C purified and low nitrogen concentration diamond combinedwith improving calibration of unknown parameters,the ODMR spectral line width can be further decreased below 0.5 MHz,corresponding to~0.18 G minimum resolvable magnetic field modulus.

关键词： vector magnetometry NV ensembles optically detected magnetic resonance(ODMR) zero bias magnetic field

Regulation of the quantum barrier and carrier transport toward high-efficiency quasi-2D Dion-Jacobson tin perovskite solar cells

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Journal of Energy Chemistry 2024年第8期95卷 200-207,I0005页

作者： Huanhuan Yao Chang Shi Tai Wu Shurong Wang Mingyu Yin Liming Ding Yong Hua Feng Hao School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871China Yunnan Key Laboratory for Micro/Nano Materials&Technology School of Materials and EnergyYunnan UniversityKunming 650091YunnanChina center for excellence in Nanoscience(CAS) Key Laboratory of Nanosystem and Hierarchical Fabrication(CAS)National Center for Nanoscience and TechnologyBeijing 100190China

Quasi-2D Dion-Jacobson(DJ)tin halide perovskite has attracted much attention due to its elimination of Van der Waals gap and enhanced environmental ***,the bulky organic spacers usually form a natural quantum well structure,which brings a large quantum barrier and poor film quality,further limiting the carrier transport and device ***,we designed three organic spacers with different chain lengths(ethylenediamine(EDA),1,3-propanediamine(PDA),and 1,4-butanediamine(BDA))to investigate the quantum barrier *** and experimental characterizations indicate that EDA with short chain can reduce the lattice distortion and dielectric confinement effect,which is beneficial to the effective dissociation of excitons and the inhibition of trap-free non-radiative *** addition,EDA cation shows strong interaction with the inorganic octahedron,realizing large aggregates in precursor solution and high-quality films with improved structural ***,femtosecond transient absorption proves that EDA cations can also weaken the formation of small n-phases with large quantum barrier to achieve effective carrier transport between different ***,the quasi-2D DJ(EDA)FA_(9)Sn_(10)I_(31)solar cells achieves a 7.07%power conversion efficiency with good environment ***,this work sheds light on the regulation of the quantum barrier and carrier transport through the chain length of organic spacer for qua si-2D DJ lead-free perovskites.

关键词： Chain lengths Organic spacers Quantum well Carrier transport Lattice distortion

Inducing mitochondriopathy-like damages by transformable nucleopeptide nanoparticles for targeted therapy of bladder cancer

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National Science Review 2024年第4期11卷 216-227页

作者： Da-Yong Hou Ni-Yuan Zhang Lu Wang Mei-Yu Lv Xiang-Peng Li Peng Zhang Yue-Ze Wang Lei Shen Xiu-Hai Wu Bo Fu Peng-Yu Guo Zi-Qi Wang Dong-Bing Cheng Hao Wang Wanhai Xu NHC and CAMS Key Laboratory of Molecular Probe and Targeted Theranostics Heilongjiang Key Laboratory of Scientific Research in Urology Harbin Medical University Department of Urology Harbin Medical University Cancer Hospital CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety CAS Center for Excellence in NanoscienceNational Center for Nanoscience and Technology(NCNST) School of Chemistry Chemical Engineering & Life Science Hubei Key Laboratory of Nanomedicine for Neurodegenerative Diseases Wuhan University of Technology

Mitochondriopathy inspired adenosine triphosphate(ATP) depletions have been recognized as a powerful way for controlling tumor growth. Nevertheless, selective sequestration or exhaustion of ATP under complex biological environments remains a prodigious challenge. Harnessing the advantages of in vivo self-assembled nanomaterials, we designed an Intracellular ATP Sequestration(IAS) system to specifically construct nanofibrous nanostructures on the surface of tumor nuclei with exposed ATP binding sites,leading to highly efficient suppression of bladder cancer by induction of mitochondriopathy-like ***, the reported transformable nucleopeptide(NLS-FF-T) self-assembled into nuclear-targeted nanoparticles with ATP binding sites encapsulated inside under aqueous conditions. By interaction with KPNA2, the NLS-FF-T transformed into a nanofibrous-based ATP trapper on the surface of tumor nuclei,which prevented the production of intracellular energy. As a result, multiple bladder tumor cell lines(T24,EJ and RT-112) revealed that the half-maximal inhibitory concentration(IC50) of NLS-FF-T was reduced by approximately 4-fold when compared to NLS-T. Following intravenous administration, NLS-FF-T was found to be dose-dependently accumulated at the tumor site of T24 xenograft mice. More significantly, this IAS system exhibited an extremely antitumor efficacy according to the deterioration of T24 tumors and simultaneously prolonged the overall survival of T24 orthotopic xenograft mice. Together, our findings clearly demonstrated the therapeutic advantages of intracellular ATP sequestration-induced mitochondriopathy-like damages, which provides a potential treatment strategy for malignancies.

关键词： self-assembly nucleopeptide nanomaterial bladder cancer mitochondriopathy

Sources appointment and health risks of PM_(2.5)-bound trace elements in a coastal city of southeastern China

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Journal of Environmental Sciences 2024年第4期138卷 561-571页

作者： Ziyi Lin Xiaolong Fan Gaojie Chen Youwei Hong Mengren Li Lingling Xu Baoye Hu Chen Yang Yanting Chen Zhiqian Shao Jinsheng Chen center for excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Key Lab of Urban Environment and Health Institute of Urban EnvironmentChinese Academy ofSciencesXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China Minnan Normal University Zhangzhou 363000China

To gain a comprehensive understanding of sources and health risks of trace elements in an area of China with high population densities and low PM_(2.5)concentrations,15 trace elements(Al,K,Ca,Ti,V,Cr,Mn,Fe,Ni,Cu,Zn,As,Sn,Ba,Pb)in PM_(2.5)were monitored from December 2020 to November 2021 in a representative city,*** concentrations of trace elements in Xiamen displayed an obvious seasonal variation and were dominated by K,Fe,Al,Ca and *** on Positive Matrix Factorization analysis,source appointment revealed that the major sources of trace elements in Xiamen were traffic,dust,biomass and firework combustion,industrial manufacture and shipping *** to health risk assessment combined with the source appointment results,it indicated that the average noncarcinogenic risk was below the threshold and cancer risk of four hazardous metals(Cr,Ni,As,Pb)exceeded the threshold(10^(-6)).Traffic-related source had almost half amount of contribution to the health risk induced by PM_(2.5)-bound trace *** the dust transport period or Spring Festival period,the health risks exceeded an acceptable threshold even an order of magnitude higher,suggesting that the serious health risks still existed in low PM_(2.5)environment at certain *** risk assessment reminded that the health risk reduction in PM_(2.5)at southeastern China should prioritize traffic-related hazardous trace elements and highlighted the importance of controlling vehicles emissions in the future.

关键词： PM_(2.5)-bound trace elements Seasonal variations Source appointment Health risks Traffic-related source

Advancing neuroscience through real-time processing of big data:Transition from open-loop to closed-loop paradigms

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Zoological Research 2024年第3期45卷 518-519页

作者： Yu-Fan Wang Jiu-Lin Du Institute of Neuroscience State Key Laboratory of NeuroscienceCenter for Excellence in Brain Science and Intelligence TechnologyChinese Academy of SciencesShanghai 200031China University of Chinese Academy of Sciences Beijing 100049China School of Life Science and Technology ShanghaiTech UniversityShanghai 200031China

The brain functions as a closed-loop system that continuously generates behavior in response to the external environment and adjusts actions based on the *** research methodologies in neuroscience,especially those employed in brain imaging experiments,have mainly adopted an open-loop paradigm(Grosenick et al.,2015).Functional neural circuits are analyzed offline and subsequently tested through manipulation of neuronal activities within specific regions or with genetic *** establishing a closed-loop research paradigm,functional ensembles can be detected and tested in real time with temporal *** functional ensembles,rather than brain regions or genetically labeled neural populations,serve as fundamental units of neural networks,offering valuable insights into the dissection of neural *** closed-loop research paradigm also enables the capture of high-dimensional activities of internal brain dynamics and precise elucidation of physiological processes such as learning,decision-making,and sleep.

关键词： neural loop Transition