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Science China Chemistry 2024年第3期67卷 1000-1007页

作者： Kun Wu Pei-Wen Cheng Xin-Yi Liu Ji Zheng Xiao-Wei Zhu Mo Xie Puxin Weng Weigang Lu Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China Guangdong Rare Earth Photofunctional Materials Engineering Technology Research Center School of Chemistry and EnvironmentJiaying UniversityMeizhou 514015China

Photocatalytic aerobic oxidation reactions are largely governed by the efficiency of charge separation and subsequent reactive oxygen species(ROS) generation. Herein, we report a polarization engineering strategy to promote the charge separation and ROS generation efficiency by substituting the benzene unit with furan/thiophene in porous organic polymers(POPs). Benefiting from the extent of local polarization, the thiophene-containing POP(JNU-218) exhibits the best photocatalytic performance in aerobic oxidation reactions, with a yield much higher than those for the furan-containing POP(JNU-217) and the benzenecontaining POP(JNU-216). Experimental studies and theoretical calculations reveal that the increase of local polarization can indeed reduce the exciton binding energy, and therefore facilitate the separation of electron-hole pairs. This work demonstrates a viable strategy to tune charge separation and ROS generation efficiency by modulating the dipole moments of the building blocks in porous polymeric organic semiconductors.

关键词： porous organic polymer local polarization photocatalytic aerobic oxidation charge separation reactive oxygen species exciton binding energy

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Uncovering the coupling effect with energy-related carbon emissions and human development variety in Chinese provinces

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Journal of environmental Sciences 2024年第5期139卷 527-542页

作者： Liu Chen Yiqi Tan Gengpei Lv Weiguang Cai Xiaofeng Gao Rui Li School of Management Science and Real Estate Chongqing UniversityChongqing 400044China State Key Joint Laboratory of environment Simulation and Pollution Control(SKLESPC) School of EnvironmentTsinghua UniversityBeijing 100084China Key Laboratory of the Three Gorges Reservoir Region’s Eco-environment Ministry of EducationCollege of Environment and EcologyChongqing UniversityChongqing 400044China

Lessening energy-related carbon emissions has become a crucial measure to achieve Chinese carbon *** study is the first to construct a Difference in Carbon pressures-adjusted Human Development Index(DCHDI)model for the purpose of exploring the coupling effect between carbon emissions and human development variety from 2000 to 2019 in Chinese *** demonstrate the following.(1)The total energy-related carbon footprint of 30 provinces in China reached 10.2 billion tons in 2019,with an average annual growth rate of 6.93% over the past two decades;and the provinces with the highest carbon emissions per capita are InnerMongolia,Ningxia,and Shanxi.(2)At the provincial level,we observed that the Human Development Index(HDI),which includes life expectancy,education,and income,has been rising,while Beijing,Shanghai,and Tianjin entered the super-high HDI level before 2008.(3)The entire coupling effect of 30 Chinese provinces has been broadly fortified in the last 20 years,but the growth rate of DCHDI values in 2011-2019 has slowed down compared with that in 2000-2010;the clustering phenomenon demonstrated that this discovery is associated with historical peaks in total carbon emissions.(4)The co-ordination degree of carbon emissions per capita and HDI was verified,and 96% of the data points were found in the range of super high coupling coordination ***,this study provides the government with worthwhile guidance for decision-making and carbon reduction strategies for other countries struggling to advance human sustainable development.

关键词： Energy-related carbon emissions Human sustainable development DCHDI model Coupling effect Chinese provinces

Insights on selective Pb adsorption via O 2p orbit in UiO-66 containing rich-zirconium vacancies

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Chinese Chemical Letters 2024年第8期35卷 357-361页

作者： Yu-Hang Li Shuai Gao Lu Zhang Hanchun Chen Chong-Chen Wang Haodong Ji Eco-environment and Resource Efficiency Research Laboratory School of Environment and EnergyPeking University Shenzhen Graduate SchoolShenzhen 518055China Beijing Key Laboratory of Functional Materials for Building Structure and environment Remediation School of Environment and Energy EngineeringBeijing University of Civil Engineering and ArchitectureBeijing 100044Chin

Herein,we constructed defective UiO-66 with rich Zr vacancy structure model,in which the defective structure was verified by various ***,the Pb adsorption experiments affirmed that defective UiO-66 could display better adsorption and selective adsorption ability than that of perfect *** results of partial density of states(PDOS)and Mulliken charge population indicated that the blue shift of O 2p and Zr 4d orbit induced the electron rearrangement of atoms closed to the bonding sites,while the positive charge number of Zr atoms decreased than *** with the expansion of pore size,Pb atom was more inclined to transfer and bond with unsaturated coordination *** significantly,quantitative structure-activity relationships(QSARs)demonstrated that selective capture of Pb instead of Zn,Cu,Cd and Hg displayed by defective UiO-66 was determined jointly by bond strength,adsorption energy and electron *** work provided some theoretical direction for the purpose of the fabrication of adsorbent and the investigation of mechanism.

关键词： Selective adsorption Heavy metal Density functional theory UiO-66 Zr vacancies

Process-driven susceptibility assessment of glacial lake outburst debris flow in the Himalayas under climate change

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Advances in Climate Change Research 2024年第3期15卷 500-514页

作者： Bin ZHOU Qiang ZOU Hu JIANG Tao YANG Wen-Tao ZHOU Si-Yu CHEN Hong-Kun YAO Institute of Mountain Hazards and environment Chinese Academy of SciencesChengdu 610041China University of Chinese Academy of Sciences Beijing 100049China School of environment and Resource Southwest University of Science and TechnologyMianyang 621010China

Global warming is causing glaciers to retreat and glacial lakes to expand in the Himalayas,which amplifies the risk of glacial lake outburst debris flows(GLODFs)and poses a significant threat to downstream lives and ***,the complex interplay between GLODF occurrences and associated indicators,coupled with the lack of a comprehensive susceptibility indicator system that considers the entire GLODF process,presents a substantial challenge in assessing GLODF susceptibility in the *** study proposes a process-driven GLODF susceptibility assessment indicator system responding to climate change that considers the complete process of GLODF formation,incorporating relevant parameters about upstream,themselves,and downstream of glacial ***,to mitigate subjective factors associated with traditional evaluation methods,we developed three novel hybrid machine-learning models by integrating classic machine-learning algorithms with the whale optimization algorithm(WOA)to delineate the distribution of GLODF susceptibility in the *** the hybrid models effectively predicted the GLODFs occurrence,with the WOA-SVC model demonstrating the highest prediction *** 34%of the catchments exhibit high and very high susceptibility levels,primarily concentrated along the north and south sides of the Himalayan ridge,particularly in the eastern and central *** capturing the physical formation process of hazards,such as topographic potential(highest relative importance value of 40%),can precisely identify GLODF.A total of 128 catchments pose potential transboundary threats,with 24 classified as having a very high susceptibility level and 25 as having a high susceptibility ***,the border region between China and Nepal is a prominent hotspot for transboundary threats of *** findings can provide valuable clues for disaster prevention,mitigation,and cross-border coordination in the Himalayas.

关键词： Glacial lake outburst debris flow Susceptibility assessment Climate change Himalayas

Gram-negative bacterial diversity and evidence of international clones of multidrug-resistant strains in zoo animals

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Integrative Zoology 2024年第3期19卷 417-423页

作者： João Pedro Rueda FURLAN Micaela Santana RAMOS Fábio Parra SELLERA Irys Hany Lima GONZALEZ Patrícia Locosque RAMOS Eliana Guedes STEHLING Department of Clinical Analyses Toxicology and Food ScienceSchool of Pharmaceutical Sciences of Ribeirão PretoUniversity of São PauloRibeirão PretoBrazil Department of Internal Medicine School of Veterinary Medicine and Animal ScienceUniversity of São PauloSão PauloBrazil School of Veterinary Medicine Metropolitan University of SantosSantosBrazil coordination of Wild Fauna Secretary of EnvironmentInfrastructure and LogisticsSão PauloBrazil

Antimicrobial resistance(AMR)is a growing phenomenon that poses a major public health challenge worldwide(Dhingra et al.2020;Antimicrobial Resistance Collaborators 2022).The selective pressure exerted in clinical settings has contributed to the longlasting successful dissemination of multidrug-resistant(MDR)Gram-negative bacteria in these environments(Chia et al.2020).

关键词： multidrug clinical

A weak but inert hindered urethane bond for high-performance dynamic polyurethane polymers

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Chinese Chemical Letters 2024年第5期35卷 238-243页

作者： Fangzhou Wang Wentong Gao Chenghui Li State Key Laboratory of coordination Chemistry School of Chemistry and Chemical EngineeringCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023China School of Materials Science and Engineering Nanjing Institute of TechnologyNanjing 211167China

Covalent adaptable networks(CANs),which share the properties of both thermosets and thermoplastics at the same time,are desirable for many *** bulky substituents is a feasible way to design dynamic covalent bonds for constructing CANs,as evidenced by the successful implementation in CANs based on hindered urea bonds(HUBs).However,the dynamicity induced by introducing bulky substituents always come with low bond energy,resulting in low mechanical strength and poor stability of the ***,we designed a novel hindered urethane bond,which is weak in thermodynamic(K_(eq)=1701.23 L/mol at 25℃)and inert in kinetic at low temperature,but stable in thermodynamic(K_(eq)=1.54×10^(4) L/mol at 100℃)and active in kinetic at high temperature(k_(-1)=0.105 h^(-1) at 80℃ and 0.315 h^(-1) at 120℃).As a result,the polyurethane based on it exhibits high mechanical properties(with Youngs’modulus of 1011±29MPa and flexible modulus reached 1833±50MPa)and excellent reversibility(can be reprocessed at 60℃ under 100 kPa in 30 min and completely healed at 40℃ in 10 min).Moreover,unlike to many CANs based on hindered urea bonds,our dynamic polyurethanes are highly stable in humid environment or even water solutions due to the slow hydrolysis *** highperformance dynamic polyurethane polymers are attractive for many applications.

关键词： Covalent adaptable networks Urethane bond Kinetics Thermodynamics

Reconstruction of biomimetic ionic channels within covalent organic frameworks for ultrafast and selective uranyl capture

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Science China Chemistry 2024年第10期67卷 3423-3431页

作者： Cheng-Rong Zhang Xiao-Juan Chen Cheng-Peng Niu Cheng Meng Shun-Mo Yi Xin Liu Jia-Xin Qi Qiu-Xia Luo Ru-Ping Liang Jian-Ding Qiu State Key Laboratory of Nuclear Resources and environment East China University of Technology College of Chemistry and Chemical Engineering Nanchang University

The efficient extraction of uranium, as the primary component of nuclear energy, holds significant implications. Drawing inspiration from the charge interaction observed in biological ion channels, we encapsulated negatively charged polystyrene sulfonate(PSS) or sodium polystyrene carboxylate(PVBA) into the nanochannels of amidoxime functionalized covalent organic framework(COF-AO) in-situ to alter the cavity environment of COF-AO. The synthesized COF-AO-PSS and COF-AO-PVBA are used for ultra-fast and highly selective uranium recovery. The negatively charged PSS/PVBA was confined in the COF-AO channel providing the driving force for uranium transport and blocking other ions, thus creating a highly selective “uranium highway”. Additionally, introducing sulfonate groups or carboxyl groups into COF-AO offers supplementary coordination environments and weak interactions with uranium. Due to charge-assisted migration and various interaction mechanisms, both COF-AO-PSS and COF-AO-PVBA exhibit faster adsorption kinetics and higher selectivity compared to COF-AO alone. Their adsorption capacities are 3.8 times and 2.4 times that of COF-AO alone respectively which highlights the necessity for constructing biomimetic ion channels in uranium adsorption processes. This work presents a bionic adsorbent based on covalent organic frameworks(COFs) for the first time, overcoming environmental and equipment limitations associated with traditional photocatalysis and electrocatalysis methods for uranium capture, opening up new avenues for designing multifunctional materials that mimic biological systems.

关键词： covalent organic frameworks Uranium biomimetic ion-channels adsorption

Self-doping active sites in microbe-derived carbonaceous electrocatalysts for the oxygen reduction reaction performance

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Nano Research 2024年第8期17卷 6803-6819页

作者： Xiaofeng Xiao Xiaochun Tian Junpeng Li Fan Yang Rui Bai Feng Zhao Key Laboratory of Urban Pollutant Conversion Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China

Microorganisms are rich in heteroatoms,which can be self-doped to form active sites during pyrolysis and loaded on microbederived carbonaceous *** recent years,microbe-derived carbonaceous materials,characterized with abundant selfdoping sites,have been continuously developed as cost-effective electrocatalysts for oxygen reduction reaction(ORR).To fully unlock the catalytic potential of microbe-derived carbonaceous materials,a comprehensive analysis of catalytic sites and mechanisms for ORR is *** paper provides a summary of the ORR catalytic performance of microbe-derived carbonaceous materials reported to date,with a specific focus on the self-doping sites introduced during their pyrolytic *** highlights the mono-or co-doping sites involving nonmetallic elements such as oxygen(O),nitrogen(N),phosphorus(P),and sulfur(S)atoms,as well as covers the doping of metallic iron(Fe)atoms with various coordination configurations in microbe-derived carbonaceous *** the impact of these self-doping sites on ORR catalytic performance can guide the design of doping sites in microbe-derived carbonaceous *** approach has the potential to maximize electrocatalytic activity of microbe-derived carbonaceous materials and contributes to the development of more efficient and cost-effective carbonaceous electrocatalysts.

关键词： electrocatalysis heteroatoms self-doped single atom catalyst microbe-derived carbonaceous material

Renewable biomass reinvigorates sustainable water-energy nexus

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Science Bulletin 2024年第16期69卷 2543-2554页

作者： Hongxu Chen Jiatao Xu Zhiyong Jason Ren Hailong Lin Leli Zhang EReaihan Yanhao Yuan Zihan Wang Zhidan Liu Laboratory of environment-Enhancing Energy(E2E) College of Water Resources and Civil EngineeringChina Agricultural UniversityBeijing 100083China Key Laboratory of Agricultural Engineering in Structure and environment Ministry of Agriculture and Rural AffairsBeijing 100083China Department of Civil and environmental Engineering Princeton UniversityPrinceton NJ 08544USA Andlinger Center for Energy and the environment Princeton UniversityPrinceton NJ 08544USA Department of Earth and environmental Engineering Columbia UniversityNew York NY 10027USA State Key Laboratory of Efficient Utilization of Agricultural Water Resources Beijing 100083China

The water-energy nexus has garnered worldwide *** dual-functional research aimed at coproducing freshwater and electricity faces significant challenges,including sub-optimal capacities("1+1coordination,high carbon footprints,and large *** water-toelectricity conversions are often compromised owing to functionality separation and erratic ***,we present a sustainable strategy based on renewable biomass that addresses these issues by jointly achieving competitive solar-evaporative desalination and robust clean electricity *** hydrothermally activated basswood,our solar desalination exceeded the 100% efficiency bottleneck even under reduced solar *** simple size-tuning,we achieved a high evaporation rate of 3.56 kg h^(-1)m^(-2)and an efficiency of 149.1%,representing 128%-251% of recent values without sophisticated surface *** incorporating an electron-ion nexus with interfacial Faradaic electron circulation and co-ion-predominated micro-tunnel hydrodynamic flow,we leveraged free energy from evaporation to generate long-term electricity(0.38 W m^(-3)for over 14 d),approximately 322% of peer performance *** inter-functional nexus strengthened dual functionalities and validated general engineering *** presented strategy holds significant promise for global human–society–environment sustainability.

关键词： Biomass Water-energy nexus Solar desalination Clean energy Hydrothermal carbonization Sustainable development

An Interfacial Gel Electrode Patch with Tunable Hydrogen Bond Network for Electromyographic Sensing and Discrimination

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CCS Chemistry 2024年第2期6卷 450-464页

作者： Jianliang Li Zhihao Liu Yongtao Tang Jiabao Xian Chaofan He Hao Wu Mingjie Liu Fengyu Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsSu Bingtian Center for Speed Research and TrainingJinan UniversityGuangzhou 510632 School of Chemistry Beihang UniversityBeijing 100191

The sensitivity and fidelity of surface electromyography(sEMG)signal monitoring is critical for muscle status and fatigue assessment,prosthetic control,and gesture ***,the incompatible skin-electrode interface and complex electrophysiological environment restrict the sensitive acquisition and accurate analysis of sEMG *** on the impedance of the skin-electrode interface issue,we developed an interfacial gel electrode patch with a tunable hydrogen bond network to simultaneously achieve a conformal interface,suitable adhesion,and high conductivity for sEMG signal *** exploiting hydroxyethylidene diphosphonic acid(HEDP)and 2-hydroxyphosphono-acetic acid(HPAA)as hydrogen bonding regulators were introduced into the polyvinyl alcohol(PVA)-based hydrogel network to regulate the hydrogen bond cross-linking *** a result,the balance of elastic modulus,adhesion,and electrical conductivity of PVA-HEDP-HPAA(PHH)hydrogel are *** reliable electrodeskin interface is manipulated to achieve conformal contact by matching the elastic modulus,reducing the gap of electrode-skin interface by adhesion,and promoting ion and electron conduction by electrical *** PHH electrode patches exhibit a lower interfacial impedance(12.56 kΩ)and a signal-to-noise ratio of 38.09±1.28 dB for accurate analysis of muscle strength and evaluation of the fatigue *** the assistance of the artificial neural network algorithm,seven gestures can be recognized with 100%prediction *** interfacial gel electrode patch contributes a bio-matching electrophysiological platform for prosthetic control,human–machine interaction,and clinical or athletic auxiliary monitoring.

关键词： hydrogel electrode hydrogen bond network surface electromyography muscle fatigue artificial neural network gesture recognition