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The remarkable but varied photosensitized oxidation by atmospheric humic-like substances at the air-water interface

Science China Chemistry 2024年

作者： Ning Yang Chu Gong Dongmei Zhang Xufeng Gao Lifeng Han Pingqing Fu Xinxing Zhang institute of Surface-Earth System Science School of Earth System Science Tianjin University College of Chemistry Frontiers Science Center for New Organic Matter State Key Laboratory of Advanced Chemical Power SourcesKey Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Tianjin Key Laboratory of Biosensing and Molecular Recognition Renewable Energy Conversion and Storage Center (ReCAST) Nankai University State Key Laboratory of component-Based Chinese Medicine Haihe Laboratory of Modern Chinese Medicine Tianjin University of Traditional Chinese Medicine

Humic-like substances(HULIS), a class of macromolecular photosensitizers, are major components of light-absorbing aerosols in the atmosphere. Due to the amphiphilic nature of HULIS, they tend to appear at the air-water interface of atmospheric ***, there have been limited studies on the photosensitized chemistry of HULIS at the air-water interface owing to the lack of methods with high interface selectivity. Here, a unique field-induced droplet ionization mass spectrometry(FIDI-MS)technique was used to investigate the photosensitized chemistry of several samples at the air-water interface. These samples include commercially available humic acid and the PM2.5sample collected during Beijing′s severe winter haze in December2016. Ultrahigh-resolution Fourier transform-ion cyclotron resonance mass spectrometry(FT-ICR MS) was also applied to analyze the atomic compositions, the degree of unsaturation and the aromaticity of these samples. Both Type I and Type II photosensitized oxidation pathways were observed, which were postulated to be dictated by the packing density of the molecules at the air-water interface. These findings reveal that the photosensitization of HULIS at the air-water interface contributes greatly to the formation of atmospheric aerosols, further advancing our understanding of the important roles played by photosensitized chemistry in the atmosphere.

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Hydrogen self-supplying initiators excited by visible light for the fabrication of transparent films

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Science China Chemistry 2024年第11期67卷 3868-3874页

作者： Qingze Pan Chiheng Liu Wenzhe Qiao Jianwei Li Saihe Yang Yangyang Xin Pengzhong Chen Jiangli Fan Xiaojun Peng State Key Laboratory of Fine Chemicals Frontiers Science Center for Smart Materials Oriented Chemical Engineering Dalian University of Technology Ningbo institute of Dalian University of Technology Key Lab of Organic Optoelectronics and Molecular Engineering of Ministry of Education Department of Chemistry Tsinghua University Liaoning Binhai Laboratory

Unimolecular Type Ⅱ radical photoinitiators(PIs) have received significant attention in photocuring owing to the fact that they improve the sustainability of the overall process compared with traditional Type Ⅱ radical photoinitiators. However, the photopolymerization efficiency of unimolecular Type Ⅱ radical photoinitiators is hindered by their short excitation wavelengths,poor photon capture abilities, and inefficient photobleaching performance. Herein, we report a coumarin-based self-sufficient initiator(C-NA), which is designed by integrating “hydrogen donor” and “hydrogen acceptor” into the coumarin framework and used for single-component visible light curing. C-NA exhibits a visible light absorbance and high molar extinction coefficient and is completely photobleached under the irradiation of 405 nm light-emitting diodes(LEDs). The formation of free radicals arises from the transfer of hydrogen from the diethylamino group to the coumarin framework, together with a highly efficient photodegradation process of C-NA. Finally, C-NA was successfully applied to prepare a transparent film material. Therefore,C-NA offers new insights into the design of promising unimolecular Type Ⅱ radical photoinitiators for photocuring.

关键词： photocuring photoinitiator hydrogen transfer visible light unimolecular photobleaching

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Tungsten chalcogenides as anodes for potassium-ion batteries

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Tungsten 2024年第2期6卷 278-292页

作者： Yu-Han Wu Wei-Hao Xia Yun-Zhuo Liu Peng-Fei Wang Yu-Hang Zhang Jin-Ru Huang Yang Xu De-Ping Li Li-Jie Ci School of Environmental and Chemical Engineering Shenyang University of TechnologyShenyang 110870China Key Laboratory of Advanced Energy materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China State Key Laboratory of Advanced Welding and Joining School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055China Department of Chemistry University College LondonLondon WC1H 0AJUnited Kingdom

Potassium-ion batteries(PIBs)by virtue of their strong cost competitiveness and similar electrochemical properties to lithiumion batteries have been deemed to be a promising electrochemical energy storage *** promote the application in the commercial market,developing electrode materials with high specifi c capacities,superior cycling stability,and reliable safety is of great *** materials as an important component of PIBs play a decisive role,among which twodimensional transition metal chalcogenides(2D TMCs)have attracted wide attention owing to their unique material and electrochemical *** the 2D TMCs’family,molybdenum chalcogenides as fl agship are the most studied materials and demonstrated the potential as *** the deepening of research on 2D TMCs,another shining member that possesses similar properties to molybdenum chalcogenides,tungsten chalcogenides(WS_(2),WSe_(2),and WTe_(2)),has aroused tremendous *** many inspiring results,various challenges remain to be further addressed;meanwhile,some results are still unclear and ***,this review fi rst introduces their material properties and electrochemical storage ***,we systematically overview the research progress and put forward promoting improvement ***,challenges and opportunities that would be future research directions are discussed.

关键词： Electrochemical energy storage Potassium-ion batteries Anodes Tungsten chalcogenides

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Dielectric response of ANb_(2)O_(6)(A = Zn, Co, Mn, Ni) columbite niobates: From microwave to terahertz

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Journal of Advanced Ceramics 2024年第8期13卷 1189-1197页

作者： Weijia Luo Shun Wang Siyong Zheng Jining Li Menglong Wang Yongzheng Wen ingxia Li Ji Zhou State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China institute of Laser and Optoelectronics School of Precision Instrument and Opto-Electronics EngineeringTianjin UniversityTianjin 300072China Shandong Inspur Artificial Intelligence Research institute Co. Ltd.Jinan 250013China School of Microelectronics Tianjin UniversityTianjin 300072China

In the upcoming 6-generation(6G)revolution,the achievement of low power consumption has become a key objective in research concerning terahertz *** an important component of passive devices,there are very few low-loss dielectric ceramics in the terahertz *** elucidate the mechanism of loss and promote the application of microwave dielectric ceramics for future 6G technology(covering microwave and terahertz frequencies),the terahertz responses of ANb_(2)O_(6)(A=Zn,Co,Mn,and Ni)columbite niobates were *** influences of magnetic loss on the Qxf values in the microwave range with different transition metal ions in the A-site were reasonably ***,due to the weakened magnetic relaxation properties in the terahertz range,the samples all exhibited low loss and approximate transparency,especially for MnNb_(2)O_(6) and NiNb_(2)O_(6)(tano<0.01 and absorption coefficient<10 cm^(-1) below 1.2 THz),which subverted the definition of traditional low-loss microwave dielectric ***,based on Mie theory,we designed a prototypical broadband metamaterial reflector to validate the applicability of the ANb_(2)O_(6) system in the terahertz band,which is highly important for the development of terahertz ceramic-based passive devices.

关键词： columbite niobates terahertz response transition metal ions magnetic loss ceramic-based metamaterials

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探索Bi_(2)SeO_(5)的高介电性能:从块体到双层和单层

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Science China materials 2024年第3期67卷 906-913页

作者：董欣月何育彧管乐祝元昊吴金雄付会霞颜丙海 Tianjin Key Lab for Rare Earth materials and Applications Center for Rare Earth and Inorganic Functional MaterialsSmart Sensor Interdisciplinary Science CenterSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China Center of Quantum materials and Devices College of PhysicsChongqing UniversityChongqing 401331China Chongqing Key Laboratory for Strongly Coupled Physics Chongqing UniversityChongqing 401331China Department of Condensed Matter Physics Weizmann Institute of ScienceRehovot 7610001Israel

Bi_(2)SeO_(5)是一种具有优异电绝缘性能的范德华(vdW)层状介电材料,引起了极大关注.然而,目前关于Bi_(2)SeO_(5)的研究主要停留在实验层面,仍然缺乏对其原子级薄膜的介电性能的相关理论认识.本文通过第一性原理计算确定了Bi_(2)SeO_(5... 详细信息

Bi_(2)SeO_(5)是一种具有优异电绝缘性能的范德华(vdW)层状介电材料,引起了极大关注.然而,目前关于Bi_(2)SeO_(5)的研究主要停留在实验层面,仍然缺乏对其原子级薄膜的介电性能的相关理论认识.本文通过第一性原理计算确定了Bi_(2)SeO_(5)的介电性能,发现其块体、双层和单层均具有超高平均介电常数(εr>20).研究表明,单层Bi_(2)SeO_(5)与双层Bi_(2)O_(2)Se之间的导带和价带能量偏移量均大于1 eV,表明单层Bi_(2)SeO_(5)依然可作为原子薄Bi_(2)O_(2)Se的良好介电层.此外,不同于h-BN或其他2D vdW绝缘体,Bi_(2)SeO_(5)的εr由其离子部分主导,且随着厚度的减小几乎保持不变.计算发现,单层Bi_(2)SeO_(5)的等效氧化层厚度可薄至0.3 n m,且单层Bi_(2)SeO_(5)在拉伸或压缩应变达到6%时均能保持高介电常数,这极大地促进了它与各种二维半导体的集成.本工作证明单层Bi_(2)SeO_(5)可以作为高性能二维电子器件良好的封装和介电层.

关键词： Bi_(2)SeO_(5) high-κ equivalent oxide thickness dielectric constant van der Waals first-principles calculations

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Boosting kinetic separation of ethylene and ethane on microporous materials via crystal size control

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Chinese Journal of Chemical Engineering 2024年第1期65卷 85-91页

作者： Yixuan Ma Cong Yu Lifeng Yang Rimin You Yawen Bo Qihan Gong Huabin Xing Xili Cui Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310012China Fundamental Science&Advanced Technology Lab PetroChina Petrochemical Research InstituteChina National Petroleum CorporationBeijing 102200China ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang UniversityHangzhou 311200China Shanxi-Zheda institute of Advanced materials and Chemical Engineering Hangzhou 310027China

The adsorptive separation of C_(2)H_(4)and C_(2)H_(6),as an alternative to distillation units consuming high energy,is a promising yet challenging *** great similarity in the molecular size of C_(2)H_(4)and C_(2)H_(6)brings challenges to the regulation of adsorbents to realize efficient dynamic ***,we reported the enhancement of the kinetic separation of C_(2)H_(4)/C_(2)H_(6)by controlling the crystal size of ZnAtzPO_(4)(Atz=3-amino-1,2,4-triazole)to amplify the diffusion difference of C_(2)H_(4)and C_(2)H_(6).Through adjusting the synthesis temperature,reactant concentration,and ligands/metal ions molar ratio,ZnAtzPO4 crystals with different sizes were *** single-component kinetic adsorption tests and binary-component dynamic breakthrough experiments confirmed the enhancement of the dynamic separation of C_(2)H_(4)/C_(2)H_(6)with the increase in the crystal size of ZnAtzPO_(4).The separation selectivity of C_(2)H_(4)/C_(2)H_(6)increased from 1.3 to 98.5 with the increase in the crystal size of ZnAtzPO_(4).This work demonstrated the role of morphology and size control of adsorbent crystals in the improvement of the C_(2)H_(4)/C_(2)H_(6)kinetic separation performance.

关键词： Adsorption Adsorbent Ethylene Binary mixture Crystal size control Kinetic separation

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The Potential Game-Changer:A Concept-to-Proof Study on D:A Heterojunction-Free Organic Photovoltaics

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Chinese Journal of Chemistry 2024年第3期42卷 252-258页

作者： Lijian Zuo Sae Byeok Jo Xueliang Shi Francis Lin Alex Jen State Key Laboratory of Silicon and Advanced Semiconductor materials MOE Key Laboratory of Macromolecular Synthesis and FunctionalizationDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhouZhejiang310058 China Department of materials Science and Engineering University of WashingtonSeattleWAUSA School of Chemical Engineering Sungkyunkwan University (SKKU)Suwon16419 Republic of Korea School of Chemistry and Molecular Engineering East China Normal UniversityShanghai200062 China Department of materials Science and Engineering City University of Hong KongKowloonHong KongChina Department of Chemistry City University of Hong KongKowloonHong KongChina Hong Kong institute for Clean Energy Hong KongChina

Since 1986,the donor-acceptor (D:A) heterojunction has been regarded a necessity for high-efficiency organic photovoltaics (OPVs),due to its unique advantage in compensating the intrinsic limitations of organic semiconductors,such as high exciton binding energy and poor ambipolar charge mobility. While this adversely causes tremendous non-radiative charge recombination and instability issues,which currently become the most critical limits for commercialization of OPVs. Here,we present a concept-to-proof study on the potential of D:A heterojunction free OPV by taking advantage of recent progress of non-fullerene acceptors. First,we demonstrate that the “free carriers” can be spontaneously generated upon illumination in an NFA,i.e.,the 6TIC-4F single layer. Second,the 6TIC-4F layer also exhibits good ambipolar charge transporting property. These exceptional characteristics distinguish it from the traditional organic semiconductors,and relieve it from the reliance of D:A heterojunction to independently work as active layer. As a result,the subsequent OPV by simply sandwiching the 6TIC-4F layer between the cathode and anode yields a considerably high power conversion efficiency ~1%. Moreover,we find the D:A heterojunction free device exhibits two order of magnitude higher electroluminescence quantum efficiency and significantly reduced VOC loss by 0.16 eV compared to those of the D:A BHJ structure,validating its promise for higher efficiency in the future. Therefore,our work demonstrates the possibility of using D:A heterojunction-free device structure for high performance,that can potentially become the next game changer of OPV.

关键词： Organic solar cells Spontaneous charge generation Ambipolar charge transport Charge recombination Perovskite-like organic semiconductor Schottky-junction structure Single component

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Nitrogen‑Doped Magnetic‑Dielectric‑Carbon Aerogel for High‑Efficiency Electromagnetic Wave Absorption

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Nano-Micro Letters 2024年第1期16卷 313-327页

作者： Shijie Wang Xue Zhang Shuyan Hao Jing Qiao Zhou Wang Lili Wu Jiurong Liu Fenglong Wang Key Laboratory for Liquid‑Solid Structural Evolution and Processing of materials Ministry of Education Shandong UniversityJinan 250061People’s Republic of China School of Mechanical Engineering Shandong UniversityJinan 250061People’s Republic of China Shenzhen Research institute of Shandong University Shenzhen 518057GuangdongPeople’s Republic of China

Carbonbased aerogels derived from biomass chitosan are encountering a flourishing moment in electromagnetic protection on account of lightweight,controllable fabrication and ***,developing a facile construction method of component design with carbon-based aerogels for high-efficiency electromagnetic wave absorption(EWA)materials with a broad effective absorption bandwidth(EAB)and strong absorption yet hits some ***,the nitrogen-doped magnetic-dielectric-carbon aerogel was obtained via ice template method followed by carbonization treatment,homogeneous and abundant nickel(Ni)and manganese oxide(MnO)particles in situ grew on the carbon *** to the optimization of impedance matching of dielectric/magnetic components to carbon aerogels,the nitrogen-doped magnetic-dielectric-carbon aerogel(Ni/MnO-CA)suggests a praiseworthy EWA performance,with an ultra-wide EAB of 7.36 GHz and a minimum reflection loss(RLmin)of−64.09 dB,while achieving a specific reflection loss of−253.32 dB mm−***,the aerogel reveals excellent radar stealth,infrared stealth,and thermal management ***,the high-performance,easy fabricated and multifunctional nickel/manganese oxide/carbon aerogels have broad application aspects for electromagnetic protection,electronic devices and aerospace.

关键词： Electromagnetic wave absorption Wide bandwidth Dielectric-magnetic synergy Multifunction

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The adsorption effect of aquaculture residual feed on heavy metals and its impact on microbial metabolism of feed

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Ecological Processes 2024年第2期13卷 246-259页

作者： Sufeng Wang Zijng Wang Wen Zhang Jingshan Li Mingyang Lin Li Chen State Key Laboratory of Metastable materials Science and Technology Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse Yanshan University Key Laboratory of Pollution Exposure and Health Intervention of Zhejiang Province College of Biology and Environmental EngineeringZhejiang Shuren University Hebei Ocean & Fisheries Science Research institute

Background Intensive and large-scale aquaculture has a high biological density, and a large amount of artificial feed must be provided. As a result, residual feed would be discharged into natural water bodies with water exchange. Due to heavy metal pollution in surface water, residual feed may adsorb heavy metals in the water, affecting the subsequent microbial degradation of feed and the restoration of the water environment. The combined ecological impacts of these two types of pollution urgently need to be *** This study explored the adsorption effect of residual feed on heavy metals and its impact on microbial degradation of residual feed. The results showed that both the insoluble component（mainly fiber, ash, and ether extract, abbreviated as FAE） and soluble component（soluble protein and starch） of the feed had adsorption effects on heavy metals. As the salinity increased, the adsorption capacity of Cu2+and Cd2+decreased, while the adsorption effect on Pb2+was not changed significantly. The adsorption of heavy metals by residual feed could affect the biological degradation of residual feed. The residual feed could adsorb heavy metals and bacterial cells simultaneously, forming FAE-B（bacteria）-S（starch）-Pr（protein）-metal adsorption complex. This adsorption effect could reduce the negative impact of heavy metals on microbial degradation of residual feed. The simulated degradation experiments in actual water bodies also confirmed this. However, the accumulation of heavy metals in residual feed may bring negative effects, such as being consumed by aquatic organisms and entering the food *** The results of this study provide a basis for the collection and centralized treatment of residual feed in aquaculture, as well as the control and remediation of residual feed pollution in natural water bodies.

关键词： Residual feed Adsorption complex Feed pollution Heavy metal

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A Web-like Three-dimensional Binder for Silicon Anode in Lithium-ion Batteries

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Energy & Environmental materials 2024年第1期7卷 21-27页

作者： Liyuan Li Tao Li Yifan Sha Baozeng Ren Lan Zhang Suojiang Zhang CAS Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Langfang Green Industrial Technology Center Langfang 065001China Henan Key Laboratory of Energy Storage materials and Processes Zhengzhou Institute of Emerging Industrial TechnologyZhengzhou 450003China

Si anode is of paramount importance for advanced energy-dense lithium-ion batteries(LIBs).However,the large volume change as well as stress generates during its lithiation-delithiation process poses a great challenge to the long-term cycling and hindering its *** this work,a composite binder is prepared with a soft component,guar gum(GG),and a rigid linear polymer,anionic polyacrylamide(APAM).Rich hydroxy,carboxyl,and amide groups on the polymer chains not only enable intermolecular crosslinking to form a web-like binder,A2G1,but also realize strong chemical binding as well as physical encapsulating to Si *** resultant electrode shows limited thickness change of merely 9%on lithiation and almost recovers its original thickness on *** demonstrates high reversible capacity of 2104.3 mAh g^(-1)after 100 cycles at a current density of 1800 mA g^(-1),and in constant capacity(1000 mAh g^(-1))test,it also shows a long life of 392 ***,this soft-hard combining web-like binder illustrates its great potential in the future applications.

关键词： anionic polyacrylamide lithium-ion batteries Si anode thickness change web-like binder

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