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Science China Chemistry 2024年

作者： Yun-Dong Cao Yuxi Zhang jian song Hong Liu Zhiyuan song Lin-Lin Fan Cai-Li Lv Guang-Gang Gao School of Materials Science and Engineering University of Jinan

The major impediment to the additional industrialization of water splitting is the high cost of the co-catalyst made of noble metals and the sacrificial reagent.A binary photocatalytic system,consisting of B-doped g-C3N4nanosheets (Cu20@BCN-X) and atomically accurate copper clusters,is designed in this *** copper clusters serve as co-catalysts for H2evolution and exhibit Pt-like activity,whereas the nanosheets serve as carriers and semiconductor components for *** binary system,created using simple techniques,demonstrates hydrogen bonding interactions that promote synergistic effects and efficient binding and charge transfer across the interface between the two *** position manipulation of carbon nitride nanosheets demonstrates a Z-scheme charge transfer mechanism between the nanosheets and copper *** photocatalytic system can accomplish the photocatalytic overall water splitting process (259.9μmol g-1h-1of H2and129.4μmol g-1h-1of O2) without using sacrificial agents or noble metal *** work lays the foundation for the design of overall water splitting catalysts by precisely manipulating the energy levels,and it also paves the way for commercialized photocatalytic catalysts that do not require noble metals or sacrificial chemicals.

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Ultra-highly selective recognition of nucleosides over nucleotides by rational modification of tetralactam macrocycle and its application in enzyme assay

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Chinese Chemical Letters 2024年第6期35卷 274-278页

作者： Huan Yao jian Qin Yan-Fang Wang song-Meng Wang Liu-Huan Yi Shi-Yao Li Fangfang Du Liu-Pan Yang Li-Li Wang School of Pharmaceutical Science Postdoctoral Research Station of Basic MedicineHengyang Medical SchoolUniversity of South ChinaHengyang 421001China Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China

Artificial macrocycle with high binding selectivity in water is often challenging but urgently needed in various research and application ***,we report a new water-soluble biomimetic tetralactam macrocycle and realize the ultra-high selectivity to nucleosides over corresponding monophosphate nucleotides by rational *** introduction of charged groups at the periphery of endofunctionalized cavity makes the selectivity(guanosine to guanosine 5-monophosphate)increase remarkably from 100 to *** on the ultra-high selectivity of biomimetic tetralactam macrocycle,the sensitive CD73 enzyme activity assay was then achieved through product-selective fluorescence indicator displacement ***,the capability of the proposed method for inhibitor screening was successfully displayed.

关键词： Rational modification Biomimetic macrocycle Ultra-high selectivity Enzyme assay

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A N-CoSe/CoSe2-C@Cu hierarchical architecture as a current collector-integrated anode for potassium-ion batteries

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Rare Metals 2024年第8期43卷 3702-3712页

作者： Zi-Jie Mu Yan-Jun Gao Wen-Shuai Dong Zong-You Li Qing-Yi song Han-Jiao Huang Li-Dong Xing jian-Guo Zhang Wei Wang Qi-Yao Yu State Key Laboratory of Explosion Science and Technology School of Mechatronical EngineeringBeijing Institute of Technology School of Metallurgical and Ecological Engineering University of Science and Technology Beijing

The highly reversible insertion/extraction of large-radius K+into electrode materials remains a tough goal,especially for con version-type ***,we design a current collector-integrated electrode（N-CoSe/CoSe2-C@Cu） as an advanced anode for potassium-ion battery（PIBs）.The conductive CoSe/CoSe2heterojunction with rich Se vacancy defects,conductive sp2N-doped carbon layer,and the elastic copper foil matrix can greatly accelerate the electron transfer and enhance the structural ***,the well-designed N-CoSe/CoSe2-C@Cu current collector-integrated electrode displays enhanced potassium storage performance with regard to a high capacity(325.1 mAh·g-1at 0.1 A·g-1after 200cycles),an exceptional rate capability(223.5 mAh·g-1at2000 mA·g-1),and an extraordinary long-term cycle stability(a capacity fading of only 0.019% per cycle over1200 cycles at 2000 mA·g-1).Impressively,ex situ scanning electron microscopy（SEM） characterizations prove that the elastic structure of copper foil is merged into the cleverly designed N-CoSe/CoSe2-C@Cu heterostructure,which buffers the deformation of structure and volume and greatly promotes the cycle life during the potassium/depotassium process.

关键词： Potassium-ion battery Integrated collector electrode CoSe CoSe 2 Heterojunction Copper foil matrix N-doped carbon

Efficient and selective H_(2)O_(2)production through uranyl-assisted photocatalytic oxygen reduction reaction process in a uranium-organic framework

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Science China Chemistry 2024年第7期67卷 2274-2281页

作者： jianxin song Chao Liang Baoyu Li Xuemin Wang Min Lei Lisha jiang Zhenyu Li Yugang Zhang jian Xie Zuju Ma Xing Dai Yanlong Wang Shuao Wang Wei Liu School of Environmental and Materials Engineering Yantai UniversityYantai 264005China State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China School of Life and Environmental Sciences Shaoxing UniversityShaoxing 312000China School of Nuclear Science and Technology Xi’an Jiaotong UniversityXi’an 710049China

Harnessing solar energy by photocatalytically converting oxygen and water into high-value-added H_(2)O_(2)is a promising way of alleviating both environmental and energy *** is worth noting that suppressing detrimental side reactions,such as the generation of·O_(2)^(-),is a critical approach to enhancing H_(2)O_(2)***,a 2-fold interpenetrating 3D uranium-organic framework(YTU-W-1)was developed and introduced for photocatalytic H_(2)O_(2)*** material demonstrates a different photocatalytic mechanism when employing uranyl as an initiator,as compared with the conventional semiconductor photocatalytic pathway involving photo-generated charge *** from the strong hydrogen abstraction effect of the U≡O·and the direct one-step oxygen reduction pathway,YTU-W-1 exhibits enhanced photocatalytic performance for H_(2)O_(2)production with yield efficiency of 221μmol h^(-1)g^(-1).Furthermore,YTU-W-1 displays a high H_(2)O_(2)selectivity of 68%,confirmed by rotating ring-disk electrode(RRDE)*** were used to elucidate the critical role of uranyl in the photocatalytic oxygen reduction reaction for H_(2)O_(2)*** research introduces an innovative approach to photo-driven H_(2)O_(2)production,underscoring the potential for heterogeneous catalysts to engage in photocatalytic reactions independently of photogenerated charge carriers.

关键词： uranyl metal-organic frameworks oxygen reduction reaction photocatalytic H_(2)O_(2)synthesis

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Changes in posterior corneal elevation after small incision lenticule extraction for different myopic diopters

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International Journal of Ophthalmology(English edition) 2024年第3期17卷 491-498页

作者： Xiao-Tong Sun Yang Zhang Xiao-Kun Mei Nan-Nan Zheng Ling-Zhi Niu Xiao-Li Qu Ai-Ping song jian Zhuo Department of Ophthalmology the First Affiliated Hospital of Shandong First Medical UniversityShandong Provincial Qianfoshan HospitalJinan 250014Shandong ProvinceChina

●AIM:To study the changes and effect factors of posterior corneal surface after small incision lenticule extraction(SMILE)with different myopic diopters.●METHODS:Ninety eyes of 90 patients who underwent SMILE were included in this retrospective *** were allocated into three groups based on the preoperative spherical equivalent(SE):low myopia(SE≥-3.00 D),moderate myopia(-3.00 D>SE>-6.00 D)and high myopia(SE≤-6.00 D).Posterior corneal surfaces were measured by a Scheimpflug camera preoperatively and different postoperative times(1wk,1,3,6mo,and 1y).Posterior mean elevation(PME)at 25 predetermined points of 3 concentric circles(2-,4-,and 6-mm diameter)above the best fit sphere was analyzed.●RESULTS:All surgeries were completed uneventfully and no ectasia was found through the *** difference of myopia group was significant at the 2-mm ring at 1 and 3mo postoperatively(1mo:P=0.017;3mo:P=0.018).The effect of time onΔPME was statistically significant(2-mm ring:P=0.001;4-mm ring:Pring:Prior corneal stability was linearly correlated with SE,central corneal thickness,ablation depth,residual bed thickness,percent ablation depth and percent stromal bed thickness.●CONCLUSION:The posterior corneal surface changes dynamically after *** protrusion is observed on the posterior corneal surface in patients with different degrees of myopia within one year after *** has good stability,accuracy,safety and predictability.

关键词： myopia posterior corneal elevation corneal ectasia small incision lenticule extraction

Radical Arbuzov Reaction

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CCS Chemistry 2024年第5期6卷 1312-1323页

作者： Linxiang Chai jian Wang Jimin Yang Junyue Yin Zhuyong Zhang Yulu Cheng Lin Zhu Xiao-song Xue Chaozhong Li Department of Chemistry University of Science and Technology of ChinaHefeiAnhui 230026 Shanghai Institute of Organic Chemistry Chinese Academy of SciencesShanghai 200032

The Arbuzov reaction(also known as the Michaelis–Arbuzov reaction)is one of the most fundamental transformations in organic chemistry and has been extensively used for the synthesis of organophosphorus compounds for over a ***,the reaction generally requires an elevated temperature and is applicable mainly to primary alkyl halides with poor functional group *** report herein a radical alternative to the conventional nucleophilic substitution ***,new radical phosphonylation reagents,9-fluorenyl o-phenylene phosphite and benzhydryl o-phenylene phosphite,have been developed for this *** photoredox-catalyzed reaction of a wide range of alkyl bromides or iodides with 9-fluorenyl(or benzhydryl)o-phenylene phosphite followed by workup with methanol(or ethanol)provides the corresponding dimethyl(or diethyl)alkylphosphonates in satisfactory yields at room temperature under mild *** method is applicable to primary,secondary,and even tertiary alkyl iodides and bromides and exhibits an excellent functional group tolerance,thereby enabling the late-stage modification of complex molecules and rapid synthesis of phosphonate-containing natural products and drug molecules.A mechanism involving the formation and subsequentβ-scission of phosphoranyl radicals is proposed.

关键词： Arbuzov reaction radicals phosphonylation photoredox catalysis alkyl halides

Invisible vapor catalysis in graphene growth by chemical vapor deposition

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Nano Research 2024年第5期17卷 4259-4269页

作者： Xiucai Sun Xiaoting Liu Zhongti Sun Xintong Zhang Yuzhu Wu Yeshu Zhu Yuqing song Kaicheng Jia Jincan Zhang Luzhao Sun Wan-jian Yin Zhongfan Liu Center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular ScienceCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing Graphene Institute(BGI) Beijing 100095China Academy for Advanced Interdisciplinary Studies Peking UniversityBeijing 100871China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China Department of Engineering University of CambridgeCambridge CB30FAUK College of Energy Soochow Institute for Energy and Materials InnovationS(SIEMIS)Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy TechnologiesSoochow UniversitySuzhou 215006China

Vapor catalysis was recently found to play a crucial role in superclean graphene growth via chemical vapor decomposition(CVD).However,knowledge of vapor-phase catalysis is scarce,and several fundamental issues,including vapor compositions and their impact on graphene growth,are ***,by combining density functional theory(DFT)calculations,an ideal gas model,and a designed experiment,we found that the vapor was mainly composed of Cui clusters with tens of *** vapor pressure was estimated to be~10^(-12)-10^(-1)1 bar under normal low-pressure CVD system(LPCVD)conditions for graphene growth,and the exposed surface area of Cui clusters in the vapor was 22-269 times that of the Cu substrate surface,highlighting the importance of vapor *** calculations show Cu clusters,represented by Cu17,have strong capabilities for adsorption,dehydrogenation,and decomposition of *** exhibit an adsorption lifetime and reaction flux six orders of magnitude higher than those on the Cu surface,thus providing a sufficient supply of active C atoms for rapid graphene growth and improving the surface cleanliness of the synthesized *** experimental validation showed that increasing the amount of Cu vapor improved the as-synthesized graphene growth rate and surface *** study provides a comprehensive understanding of vapor catalysis and the fundamental basis of vapor control for superclean graphene rapid growth.

关键词： vapor catalysis graphene growth chemical vapor deposition first-principles calculation

Electrolytes additives for Zn metal anodes: regulation mechanism and current perspectives

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Rare Metals 2024年第9期43卷 4162-4197页

作者： Yu-Zhe Zhang Huai-Sheng Ao Qi Dong Shao-Jie Zhang Zhi-Guo Hou Na-Na Wang Xue-song Xie jian Rong Zhong-Yu Li School of Environmental Science and Engineering Changzhou University School of Petrochemical Engineering Changzhou University Hefei National Laboratory for Physical Science at Microscale School of Chemistry and Materials Science University of Science and Technology of China Institute for Superconducting and Electronic Materials Australian Institute for Innovative Materials Innovation Campus University of Wollongong Department of Chemical and Materials Engineering University of Alberta

With distinct advantages such as high gravimetric and volumetric capacity(5855 mAh·cm-3and 820mAh·g-1), low redox potential(-0.762 V vs. standard hydrogen electrode（SHE）), high abundance, low toxicity and intrinsic safety of Zn metal anode, Zn-ion batteries have become a potential alternative to Li-ion ***, several challenges still need to be addressed prior to the practical applications of Zn-ion batteries, such as dendrite growth during Zn plating/stripping and interfacial side reactions on the Zn surface. Such issues can be addressed by introducing additives to regulate the components and structures of the electrolyte. In this review, we systematically discussed the core issues of metallic Zn anodes and comprehensively summarized a novel perspective of the regulation mechanism of inhibiting dendrite growth or interfacial side reactions in Zn anodes by introducing additives into aqueous ***, some discussions and prospects for aqueous Zn ion batteries（AZIBs） are presented for future research.

关键词： AZIBs Current perspectives Electrolyte additives Regulation mechanism Zn metal anode

Programmable repulsive potential for tight-binding from ChenM?bius inversion theorem

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Science China(Physics,Mechanics & Astronomy) 2024年第1期 75-87页

作者： jian-Gao Li Jin-Kun Tang Hong-Quan song Gotthard Seifert Dong-Bo Zhang College of Nuclear Science and Technology Beijing Normal University Department of Physics Beijing Normal University College of Physics and Telecommunication Engineering Zhoukou Normal University Theoretische Chemie Technische Universit?t Dresden

An accurate total energy calculation is essential in materials computation. To date, many tight-binding(TB) approaches based on parameterized hopping can produce electronic structures comparable to those obtained using first-principles ***, TB approaches still have limited applicability for determining material properties derived from the total energy. That is, the predictive power of the TB total energy is impaired by an inaccurate evaluation of the repulsive energy. The complexity associated with the parametrization of TB repulsive potentials is the weak link in this evaluation. In this study, we propose a new method for obtaining the pairwise TB repulsive potential for crystalline materials by employing the Chen-M?bius inversion theorem. We show that the TB-based phonon dispersions, calculated using the resulting repulsive potential, compare well with those obtained by first-principles calculations for various systems, including covalent and ionic bulk materials and twodimensional materials. The present approach only requires the first-principles total energy and TB electronic band energy as input and does not involve any parameters. This striking feature enables us to generate repulsive potentials programmatically.

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Acupoint catgut-embedding therapy ameliorates DNCB-induced atopic dermatitis in BALB/c mice by regulating Th2 type immune response and reducing infiltration of CD4^(+)and CD8^(+)cells

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Traditional Medicine Research 2024年第9期9卷 14-20页

作者： Cheng Qin Xiang-Yi Kong Fang Wang Jin Xu Zhuo Zhang Xue-song Yang jian-Zhou Ye College of First Clinical Medicine Yunnan University of Traditional Chinese MedicineKunming 650500China Yunnan Key Laboratory of Dai and Yi Medicines Yunnan University of Chinese MedicineKunming 650500China Yunnan Provincial Key Laboratory of Molecular Biology for Sinomedicine Yunnan University of Chinese MedicineKunming 650500China Department of Dermatology The First Affiliated Hospital of Yunnan University of Traditional Chinese MedicineKunming 650021China

Background:This study aimed to assess how acupoint catgut-embedding therapy influences Th2-type immune response and the infiltration of CD4^(+)and CD8^(+)cells in DNCB-induced atopic dermatitis in BALB/c *** also conducted an initial examination of the underlying molecular ***:Seventy-two mice were randomly divided into four groups:normal control,DNCB-induced atopic dermatitis model(AD),AD with acupoint catgut-embedding treatment(ADA),and AD with sham-acupoint catgut-embedding *** DNCB challenge to induce AD,the ADA group received acupoint catgut-embedding therapy treatment at Zusanli(ST 36)and Quchi(LI 11)acupoints every other week from day *** in the AD with sham-acupoint catgut-embedding treatment group underwent the same procedure as the ADA group but without catgut *** was assessed using SCORAD on treatment days 1,10,and *** day 18,nine mice per group were euthanized,and the remaining on day *** changes were observed using hematoxylin-eosin and immunohistochemistry ***-α,IL-4,IL-6,and IL-13 levels were analyzed by ELISA,and GATA3 and STAT6 protein levels by western ***:After 20 days of acupoint catgut-embedding therapy treatment,mice showed reduced dermatitis scores compared to DNCB-induced AD-like *** decreases occurred in serum IL-4,IL-6,IL-13,and TNF-α*** analysis revealed marked reductions in CD4^(+)and CD8^(+)cell infiltration,as well as GATA3 and STAT6 protein ***:Acupoint catgut-embedding therapy may effectively alleviate atopic dermatitis by suppressing Th2 immune responses via the STAT6-GATA3 pathway and reducing CD4^(+)and CD8^(+)T cell infiltration in skin lesions.

关键词： atopic dermatitis acupoint catgut-embedding therapy Th2 type immune response