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Fe-doped Co_(3)O_(4) nanowire strutted 3D pinewood-derived carbon: A highly selective electrocatalyst for ammonia production via nitrate reduction

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Nano Research 2024年第4期17卷 2276-2282页

作者： Xuwei Liu Chaozhen Liu Xun He Zhengwei Cai Kai Dong Jun Li Xiaoya Fan Ting Xie Xiya Yang Yonglan Luo Dongdong Zheng Shengjun Sun Sulaiman Alfaifi Feng Gong Xuping Sun Institute of Fundamental and frontier sciences University of Electronic Science and Technology of ChinaChengdu 610054China Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing 211189China College of Chemistry Chemical Engineering and Materials ScienceShandong Normal UniversityJinan 250014China Chemistry department Frontier of ScienceKing Abdulaziz UniversityJeddah 21589Saudi Arabia

Nitrate(NO_(3)^(-)),a nitrogen-containing pollutant,is prevalent in aqueous solutions,contributing to a range of environmental and health-related issues.The electrocatalytic reduction of NO_(3)^(-)holds promise as a sustainable approach to both eliminating NO_(3)^(-)and generating valuable ammonia(NH_(3)).Nevertheless,the reduction reaction of NO_(3)^(-)(NO_(3)^(-)RR),involving 8-electron transfer process,is intricate,necessitating highly efficient electrocatalysts to facilitate the conversion of NO_(3)^(-)to NH_(3).In this study,Fe-doped Co_(3)O_(4) nanowire strutted three-dimensional(3D)pinewood-derived carbon(Fe-Co_(3)O_(4)/PC)is proposed as a high-efficiency NO_(3)^(-)RR electrocatalyst for NH_(3) production.Operating within 0.1 M NaOH containing NO_(3)^(-),Fe-Co_(3)O_(4)/PC demonstrates exceptional performance,obtain an impressively large NH_(3) yield of 0.55 mmol·h^(-1)·cm^(-2) and an exceptionally high Faradaic efficiency of 96.5%at-0.5 V,superior to its Co_(3)O_(4)/PC counterpart(0.2 mmol·h^(-1)·cm^(-2),73.3%).Furthermore,the study delves into the reaction mechanism of Fe-Co_(3)O_(4) for NO_(3)^(-)RR through theoretical calculations.

关键词： Fe-doped Co_(3)O_(4) nanowire pinewood-derived carbon electrocatalytic NO_(3)-reduction NH_(3) synthesis density functional theory

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Polyhydroxyurethanes from Biobased Monomers and CO_(2):A Bridge between Sustainable Chemistry and CO_(2) Utilization

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Chinese Journal of Chemistry 2024年第6期42卷 652-685页

作者： Tharinee Theerathanagorn Tanika Kessaratikoon Hafeez Ur Rehman Valerio D'Elia Daniel Crespy VISTEC advanced Laboratory for environment-Related Inorganic and Organic Syntheses Department of Materials Science and EngineeringVidyasirimedhi Institute of Science and Technology21210Wang ChanRayongThailand department of Materials science and Engineering Vidyasirimedhi Institute of Science and Technology21210Wang ChanRayongThailand

Polyhydroxyurethanes(PHUs)have received considerable attention in the last decade as potential alternatives to traditional phosgene-based polyurethanes(PUs).The development of suitable 5CC(five membered-ring cyclic carbonate)precursors bearing multiple carbonate moieties(multi-5CCs)is a key requisite for preparing PHUs by polyaddition reaction with bis-or polyamines.Producing sustainable PHUs from CO_(2)-based five-membered cyclic carbonates(5CCs)obtained from biobased epoxides is a valuable strategy to bridge CO_(2) utilization and the upcycling of renewable substrates.In this context,while many multi-5CC monomers reported in the literature are oil-based,recent efforts have led to the development of a large variety of multifunctional 5CCs that are produced by the combination of CO_(2) and renewable resources such as fatty acids and vegetable oils,lignin,terpenes,and sugars.In this work,recent crucial advances(2019—2023)on PHUs prepared from bis-and multi-5CCs produced from CO_(2) and(partially/potentially)biobased substrates are reviewed with respect to their synthesis,thermal and mechanical properties,and their recent,emerging applications.

关键词： CO_(2) conversion Polyhydroxyurethanes Cyclic carbonates Biobased compounds Fatty acids Functional polymers Monomers Renewable resources

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Investigating the effect of volatility on the hygroscopicities of acetate nanoparticle aerosols by surface plasmon resonance microscopy

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Journal of environmental sciences 2024年第4期138卷 167-178页

作者： Bo Yang Zhibo Xie Jianguo Liu Huaqiao Gui Jiaoshi Zhang Xiuli Wei Zetao Fan Douguo Zhang Key Laboratory of environmental Optics and Technology Anhui Institute of Optics and Fine MechanicsHefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China University of science and Technology of China Hefei 230026China CAS Center for Excellence in Regional Atmospheric environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China advanced Laser Technology Laboratory of Anhui Province Department of Optics and Optical EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Under high relative humidity(RH)conditions,the release of volatile components(such as acetate)has a significant impact on the aerosol hygroscopicity.In this work,one surface plasmon resonance microscopy(SPRM)measurement system was introduced to determine the hygroscopic growth factors(GFs)of three acetate aerosols separately or mixed with glucose at different RHs.For Ca(CH_(3)COO)_(2) or Mg(CH_(3)COO)_(2) aerosols,the hygroscopic growth trend of each time was lower than that of the previous time in three cyclic humidification from 70% RH to 90% RH,which may be due to the volatility of acetic acid leading to the formation of insoluble hydroxide(Ca(OH)_(2) or Mg(OH)_(2))under high RH conditions.Then the third calculated GF(using the Zdanovskii-Stokes-Robinson method)for Ca(CH_(3)COO)_(2) or Mg(CH_(3)COO)_(2) in bicomponent aerosols with 1:1 mass ratio were 3.20% or 5.33% lower than that of the first calculated GF at 90% RH.The calculated results also showed that the hygroscopicity change of bicomponent aerosol was negatively correlated with glucose content,especially when the mass ratio of Mg(CH_(3)COO)_(2) to glucose was 1:2,the GF at 90% RH only decreased by4.67% after three cyclic humidification.Inductively coupled plasma atomic emission spectrum(ICP-AES)based measurements also indicated that the changes of Mg^(2+)concentration in bicomponent was lower than that of the single-component.The results of this study reveal thatduring the efflorescence transitions of atmospheric nanoparticles,the organic acids diffusion rate may be inhibited by the coating effect of neutral organic components,and the particles aging cycle will be prolonged.

关键词： Hygroscopic growth Volatility Acetate aerosols Nanoparticle aerosol Surface plasmon resonance

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High-resolution multi-scale air pollution system:Evaluation of modelling performance and emission control strategies

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Journal of environmental sciences 2024年第3期137卷 65-81页

作者： Diogo Lopes Joana Ferreira Sandra Rafael Ka In Hoi Xin Li Yuan Liu Ka-Veng Yuen Kai Meng Mok Ana Isabel Miranda department of environment and Planning&CESAM University of AveiroAveiroPortugal department of Civil&environmental Engineering Faculty of Science and TechnologyUniversity of MacaoMacao SARChina

A high percentage of the world's population lives in areas where air pollutant concentrations exceed the World Health Organization guidelines.This work aims to develop and test,a high-resolution multi-scale air pollution modelling system by integrating a set of adequate tools.This system is able to provide detailed air pollutant concentrations in urban areas and support air quality management strategies through a better identification of different atmospheric processes.It also allows furthering the design and assessment of air pollution control measures for a specific area.To evaluate its performance and suitability,the system was applied to the Macao Special Administrative Region(SAR),China,one of the most densely populated areas on earth,during a winter period when this area is affected by high levels of Particulate Matter(PM).Although the developed system tends to underestimate the PM concentrations,it revealed a good performance in reproducing the temporal and spatial air pollution patterns.Several exceedances of the Chinese air quality standards were calculated and high population exposure to PM pollution was estimated.The tested urban atmospheric emission reduction scenarios have shown air quality improvements,indicating that emission reduction measures at urban level should focus on the domestic sector.However,it is crucial to implement joint pollution prevention strategies with neighbouring regions to improve the air quality in Macao SAR.The approach developed in this work can support policymakers in defining new strategies to reduce atmospheric pollution in urban areas.

关键词： Urban areas High-resolution emission inventory Particulate matter Population exposure

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Prediction and interpretation of photocatalytic NO removal on g-C_(3)N_(4)-based catalysts using machine learning

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Chinese Chemical Letters 2024年第2期35卷 477-483页

作者： Jing Li Xinyan Liu Hong Wang Yanjuan Sun Fan Dong School of Resources and environment University of Electronic Science and Technology of ChinaChengdu 611731China Research Center for Carbon-Neutral environmental & Energy Technology Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731China

Predictive modeling of photocatalytic NO removal is highly desirable for efficient air pollution abatement.However,great challenges remain in precisely predicting photocatalytic performance and understanding interactions of diverse features in the catalytic systems.Herein,a dataset of g-C_(3) N_(4)-based catalysts with 255 data points was collected from peer-reviewed publications and machine learning(ML)model was proposed to predict the NO removal rate.The result shows that the Gradient Boosting Decision Tree(GBDT)demonstrated the greatest prediction accuracy with R 2 of 0.999 and 0.907 on the training and test data,respectively.The SHAP value and feature importance analysis revealed that the empirical categories for NO removal rate,in the order of importance,were catalyst characteristics>reaction process>preparation conditions.Moreover,the partial dependence plots broke the ML black box to further quantify the marginal contributions of the input features(e.g.,doping ratio,flow rate,and pore volume)to the model output outcomes.This ML approach presents a pure data-driven,interpretable framework,which provides new insights into the influence of catalyst characteristics,reaction process,and preparation conditions on NO removal.

关键词： Machine learning g-C_(3)N_(4)-based catalysts NO removal Interpretability Catalytic informatics

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Unveiling the size effect of nitrogen-doped carbon-supported copper-based catalysts on nitrate-to-ammonia electroreduction

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Nano Research 2024年第4期17卷 2438-2443页

作者： Ran Li Taotao Gao Wenxi Qiu Minghao Xie Zhaoyu Jin Panpan Li College of Materials science and Engineering Sichuan UniversityChengdu 610065China Institute for advanced Study Chengdu UniversityChengdu 610106China Materials science and Engineering Program and Walker department of Mechanical Engineering The University of Texas at AustinAustinTexas 78712USA Institute of Fundamental and frontier sciences University of Electronic Science and Technology of ChinaChengdu 610054China

The electrocatalytic nitrate reduction reaction(NitRR)represents a promising approach toward achieving economically and environmentally sustainable ammonia.However,it remains a challenge to regulate the size effect of electrocatalysts to optimize the catalytic activity and ammonia selectivity.Herein,the Cu-based catalysts were tailored at the atomic level to exhibit a size gradient ranging from single-atom catalysts(SACs,0.15–0.35 nm)to single-cluster catalysts(SCCs,1.0–2.8 nm)and nanoparticles(NPs,20–30 nm),with the aim of studying the size effect for the NO_(3)^(-)-to-NH_(3) reduction reaction.Especially,the Cu SCCs exhibit enhanced metal–substrate and metal–metal interactions by taking advantageous features of Cu SACs and Cu NPs.Thus,Cu SCCs achieve exceptional electrocatalytic performance for the NitRR with a maximum Faradaic efficiency of ca.96%NH_(3)and the largest yield rate of ca.1.99 mg·h^(-1)·cm^(-2) at-0.5 V vs.reversible hydrogen electrode(RHE).The theoretical calculation further reveals the size effect and coordination environment on the high catalytic activity and selectivity for the NitRR.This work provides a promising various size-controlled design strategy for aerogel-based catalysts effectively applied in various electrocatalytic reactions.

关键词： nitrate electroreduction ammonia electrosynthesis size effect single-cluster catalyst

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Facet-dependent transformation and toxicity of nanoscale zinc oxide in the synthetic saliva

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Journal of environmental sciences 2024年第5期139卷 170-181页

作者： Xiang Zhang Yunpeng Huang Jikun Wang Jie Tang YangMei Nali Zhu Zhigang Li Lingxiangyu Li YaweiWang School of environment Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China College of Resources and environment University of Chinese Academy of SciencesBeijing 100049China State Key Laboratory of environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Key Laboratory of Systems Health science of Zhejiang Province Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China department of Chemistry University of PennsylvaniaPhiladelphia 19104USA

The nanoscale zinc oxide(n-ZnO)was used in food packages due to its superior antibac terial activity,resulting in potential intake of n-ZnO through the digestive system,wherein n-ZnO interacted with saliva.In recent,facet engineering,a technique for controlling the exposed facets,was applied to n-ZnO,whereas risk of n-ZnO with specific exposed facets in saliva was ignored.ZnO nanoflakes(ZnO-0001)and nanoneedles(ZnO-1010)with the pri mary exposed facets of{0001}and{1010}respectively were prepared in this study,investigat ing stability and toxicity of ZnO-0001 and ZnO-1010 in synthetic saliva.Both ZnO-0001 and ZnO-1010 partially transformed into amorphous Zn_(3)(PO_(4))_(2)within 1 hr in the saliva even containing orgnaic components,forming a ZnO-Zn_(3)(PO_(4))_(2)core-shell structure.Neverthe less,ZnO-1010 relative to ZnO-0001 would likely transform into Zn_(3)(PO_(4))_(2),being attributed to superior dissolution of{1010}facet due to its lower vacancy formation energy(1.15 eV than{0001}facet(3.90 eV)).The toxicity of n-ZnO to Caco-2 cells was also dependent on the primary exposed facet;ZnO-0001 caused cell toxicity through oxidative stress,whereas ZnO-1010 resulted in lower cells viability than ZnO-0001 through oxidative stress and mem brane damage.Density functional theory calculations illustrated that·O_(2)^(-)was formed and released on{1010}facet,yet O_(2)^(2-)instead of·O_(2)^(-)was generated on{0001}facet,leading to low oxidative stress from ZnO-0001.All findings demonstrated that stability and toxicity of n-ZnO were dependent on the primary exposed facet,improving our understanding o health risk of nanomaterials.

关键词： The exposed facet Nanoscale ZnO Chemical transformation Synthetic salica Nanotoxicity

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A systematic review of the inequality of health burdens related to climate change

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frontiers of environmental science & Engineering 2024年第5期18卷 137-153页

作者： Xinke Song Shihui Zhang Hai Huang Qun Ding Fang Guo Yaxin Zhang Jin Li Mingyu Li Wenjia Cai Can Wang State Key Joint Laboratory of environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing100084China department of Earth System science Tsinghua UniversityBeijing100084China

Climate change significantly impacts human health,exacerbating existing health inequalities and creating new ones.This study addresses the lack of systematic review in this area by analyzing 2440 publications,focusing on four key terms:health,disparities,environmental factors,and climate change.Strict inclusion criteria limited the selection to English-language,peer-reviewed articles related to climate health hazards,ensuring the relevance and rigor of the synthesized studies.This process synthesized 65 relevant studies.Our investigation revealed that recent research,predominantly from developed countries,has broadened its scope beyond temperature-related impacts to encompass diverse climate hazards,including droughts,extreme weather,floods,mental health issues,and the intersecting effects of Coronavirus Disease 2019.Research has highlighted exposure as the most studied element in the causal chain of climate change-related health inequalities,followed by adaptive capability and inherent sensitivity.The most significant vulnerabilities were observed among populations with low socioeconomic status,ethnic minorities,and women.The study further reveals research biases and methodological limitations,such as the paucity of attention to underdeveloped regions,a narrow focus on non-temperature-related hazards,challenges in attributing climate change effects,and a deficit of large-scale empirical studies.The findings call for more innovative research approaches and a holistic integration of physical,socio-political,and economic dimensions to enrich climate-health discourse and inform equitable policy-making.

关键词： Climate change Health impact Human well-being Inequality Vulnerability

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Revisiting the spin effects induced by thermal vorticity

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Chinese Physics C 2024年第5期48卷 194-208页

作者：高建华杨诗正 Shandong Key Laboratory of Optical Astronomy and Solar-Terrestrial environment School of Space Science and PhysicsShandong UniversityWeihai 264209China Institute of frontier and Interdisciplinary science Key Laboratory of Particle Physics and Particle Irradiation(MOE)Shandong UniversityQingdao 266237China

We revisit the spin effects induced by thermal vorticity by calculating them directly from the spin-dependent distribution functions.For spin-1/2 particles,we provide the polarization up to the first order of thermal vorticity and compare it with the usual results calculated from the spin vector.For spin-1 particles,we show that all the non-diagonal elements vanish and there is no spin alignment up to the first order of thermal vortcity.We present the spin alignment at second-order contribution from thermal vorticity.We also show that the spin effects for both Dirac and vector particles receive an extra contribution when the spin direction is associated with the momentum of the particle.

关键词： relativistic heavy ion collisions global polarization quark gluon plasma

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Source apportionment of PM_(2.5)using PMF combined online bulk and single-particle measurements:Contribution of fireworks and biomass burning

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Journal of environmental sciences 2024年第2期136卷 325-336页

作者： Yanjing Zhang Wenshuai Li Lei Li Mei Li Zhen Zhou Jianzhen Yu Yang Zhou frontier science Center for Deep Ocean Multispheres and Earth System(FDOMES)and Physical Oceanography Laboratory Ocean University of ChinaQingdaoShandong 266100China College of Oceanic and Atmospheric sciences Ocean University of ChinaQingdaoShandong 266100China Institute of Atmospheric environment Safety and Pollution Control Jinan UniversityGuangdong 510632China Institute of environment Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina department of Chemistry Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina Division of environment The Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina

Fireworks(FW)could significantly worsen air quality in short term during celebrations.Due to similar tracers with biomass burning(BB),the fast and precise qualification of FW and BB is still challenging.In this study,online bulk and single-particle measurements were combined to investigate the contributions of FW and BB to the overall mass concentrations of PM_(2.5)and specific chemical species by positive matrix factorization(PMF)during the Chinese New Year in Hong Kong in February 2013.With combined information,fresh/aged FW(abundant ^(140)K_(2)NO_(3)^(+)and ^(213)K_(3)SO_(4)^(+)formed from ^(113)K_(2)Cl^(+)discharged by fresh FW)can be extracted from the fresh/aged BB sources,in addition to the Second Aerosol,Vehicles+Road Dust,and Sea Salt factors.The contributions of FW and BB were investigated during three high particle matter episodes influenced by the pollution transported from the Pearl River Delta region.The fresh BB/FW contributed 39.2%and 19.6%to PM_(2.5)during the Lunar Chinese New Year case.However,the contributions of aged FW/BB enhanced in the last two episodes due to the aging process,evidenced by high contributions from secondary aerosols.Generally,the fresh BB/FW showed more significant contributions to nitrate(35.1%and15.0%,respectively)compared with sulfate(25.1%and 5.9%,respectively)and OC(14.8%and11.1%,respectively)on average.In comparison,the aged FW contributed more to sulfate(13.4%).Overall,combining online bulk and single-particle measurement data can combine both instruments’advantages and provide a new perspective for applying source apportionment of aerosols using PMF.

关键词： Source apportionment PMF Online bulk measurements Single particle analysis Fireworks Biomass burning

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