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Rapid energy Exchange between In Situ Formed Bromine Vacancies and CO_(2)Molecules Enhances CO_(2)Photoreduction

Research 2024年第2期2023卷 763-771页

作者： Qin Ren Ye He Hong Wang Yanjuan Sun Fan Dong Research center for environmental and energy catalysis Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731China School of Resources and Environment University of Electronic Science and Technology of ChinaChengdu 611731China

Photocatalytic reduction of CO_(2)into fuels provides a prospective tactic for regulating the global carbon balance utilizing renewable solar ***,CO_(2)molecules are difficult to activate and reduce due to the thermodynamic stability and chemical *** this work,we develop a novel strategy to promote the adsorption and activation of CO_(2)molecules via the rapid energy exchange between the photoinduced Br vacancies and CO_(2)*** in situ continuous wave-electron paramagnetic resonance(cw-EPR)and pulsed EPR technologies,we observe that the spin-spin relaxation time(T_(2))of BiOBr is decreased by 198 ns during the CO_(2)photoreduction reaction,which is further confirmed by the broadened EPR *** result reveals that there is an energy exchange interaction between in situ formed Br vacancies and CO_(2)molecules,which promotes the formation of high-energy CO_(2)molecules to facilitate the subsequent reduction *** addition,theoretical calculations indicate that the bended CO_(2)adsorption configuration on the surface of BiOBr with Br vacancies caused the decrease of the lowest unoccupied molecular orbital of the CO_(2)molecule,which makes it easier for CO_(2)molecules to acquire electrons and get *** situ diffuse reflectance infrared Fourier transform spectroscopy further shows that the activated CO_(2)molecules are favorably converted to key intermediates of COOH*,resulting in a CO generation rate of 9.1μmol g^(-1)h^(-1)and a selectivity of 100%.This study elucidates the underlying mechanism of CO_(2)activation at active sites and deepens the understanding of CO_(2)photoreduction reaction.

关键词： reaction. adsorption activation

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The influence of patterned microporous layer on the proton exchange membrane fuel cell performances

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Nano Research 2024年第7期17卷 6095-6101页

作者： Shunzhong Wang Kadi Hu Wei Chen Yali Cao Linan Wang Zhichang Wang Lirui Cui Mingzheng Zhou Wei Zhu Hui Li Zhongbin Zhuang State Key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China State Power Investment Corporation hydrogen energy Company Ltd.Beijing 102600China Beijing Advanced Innovation center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of energy environmental catalysis Beijing University of Chemical TechnologyBeijing 100029China

The ordered membrane electrode assembly(MEA)has gained much attention because of its potential in improving mass ***,a comprehensive study was conducted on the influence of the patterned microporous layer(MPL)on the proton exchange membrane fuel cell *** patterned MPL is employed,grooves are generated between the catalyst layer and the gas diffusion *** is found that the grooves do not increase the contact resistance,and it is beneficial for water *** the MEA works under low humidity scenarios,the MEA with patterned MPL illustrated higher performance,due to the reduced inner resistance caused by improved water retention,leading to increased ionic ***,when the humidity is higher than 80%or working under high current density,the generated water accumulated in the grooves and hindered the oxygen mass transport,leading to a reduced MEA performance.

关键词： microporous layer patterned proton exchange membrane fuel cell mass transport humidity water reduction

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Feasibility of low-intensity ultrasound treatment with hydroxylamine to accelerate the initiation of partial nitrification and allow operation under intermittent aeration

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Journal of environmental Sciences 2024年第5期139卷 446-459页

作者： Jianxiong Jian Xiaojian Liao Zhihua Mo Shoupeng Li Lei Li Shaojin Chen Zhenhua Huang Junhao Chen Wencan Dai Shuiyu Sun Guangzhou Key Laboratory environmental catalysis and Pollution Control Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlSchool of Environmental Science and EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangdong Province Solid Waste Recycling and Heavy Metal Pollution Control Engineering Technology Research center Guangdong Polytechnic of Environmental Protection EngineeringFoshan 528216China Analysis and Test center Guangdong University of TechnologyGuangzhou 510006China

Partial nitrification is a key aspect of efficient nitrogen removal,although practically it suf-fers from long start-up cycles and unstable long-term operational *** address these drawbacks,this study investigated the effect of low intensity ultrasound treatment combined with hydroxylamine(NH2OH)on the performance of partial *** showthat compared with the control group,low-intensity ultrasound treatment(0.10W/mL,15 min)combined with NH2OH(5 mg/L)reduced the time required for partial nitrification initiation by 6 days,increasing the nitrite accumulation rate(NAR)and ammonia nitro-gen removal rate(NRR)by 20.4% and 6.7%,respectively,achieving 96.48% ***-tic analysis showed that NH2OH enhanced ammonia oxidation,inhibited nitrite-oxidizing bacteria(NOB)activity and shortened the time required for partial nitrification ***,ultrasonication combined with NH2OH dosing stimulated EPS(extracellular polymeric substances)secretion,increased carbonyl,hydroxyl and amine functional group abundances and enhanced mass *** addition,16S rRNA gene sequencing results showed that ultrasonication-sensitive Nitrospira disappeared from the ultrasound+NH_(2)OH system,while Nitrosomonas gradually became the dominant ***,the results of this study provide valuable insight into the enhancement of partial nitrification start-up during the process of wastewater nitrogen removal.

关键词： Partial nitrification Low-intensity ultrasound Hydroxylamine Ammonia oxidizing bacteria Nitrite oxidizing bacteria

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Photodegradation of xylene isomers:Kinetics,mechanism,secondary pollutant formation potential and health risk evaluation

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Journal of environmental Sciences 2024年第2期136卷 658-669页

作者： Xiaoyan Chen Weikun Zhu Sufen Feng Jiangyao Chen Guangdong Key Laboratory of environmental catalysis and Health Risk Control Guangdong Technology Research Center for Photocatalytic Technology Integration and Equipment EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key Laboratory of environmental catalysis and Pollution Control Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and HealthSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Photodegradation technology has been widely applied in the purification of industrial aromatic ***,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still ***,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light *** lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 *** xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and *** them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of ***,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure ***,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded *** findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.

关键词： Isomer aromatics Photodegradation Ozone formation Secondary organic aerosols Health risk

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A weakly-solvated ether-based electrolyte for fast-charging graphite anode

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Chinese Chemical Letters 2024年第8期35卷 526-532页

作者： Xiao Zhu Yanbing Mo Jiawei Chen Gaopan Liu Yonggang Wang Xiaoli Dong Department of Chemistry and Shanghai Key Laboratory of Molecular catalysis and Innovative Materials Institute of New EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Fudan UniversityShanghai 200433China

Weakly-solvated electrolytes(WSEs)utilizing solvents with weak coordination ability offer advantages for low-potential graphite anode owing to their facile desolvation process and anions-derived inorganic-rich solid electrolyte interphase(SEI)***,these electrolytes face challenges in achieving a balance between the weak solvation affinity and high ionic conductivity,as well as between rigid inorganic-rich SEI and flexible SEI for long-term ***,we introduce 1,3-dioxolane(DOL)and lithium bis(trifluoromethanesulfonyl)-imide(LiTFSI)as functional additives into a WSE based on nonpolar cyclic ether(1,4-dioxane).The well-formulated WSE not only preserves the weakly solvated features and anion-dominated solvation sheath,but also utilizes DOL to contribute organic species for stabilizing the SEI *** from these merits,the optimized electrolyte enables graphite anode with excellent fast-charging performance(210 mAh/g at 5 C)and outstanding cycling stability(600 cycles with a capacity retention of 82.0%at room temperature and 400 cycles with a capacity retention of 80.4%at high temper-ature).Furthermore,the fabricated LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)||graphite full cells demonstrate stable operation for 140 cycles with high capacity retention of 80.3%.This work highlights the potential of tailoring solvation sheath and interphase properties in WSEs for advanced electrolyte design in graphite-based lithium-ion batteries.

关键词： Weakly-solvated solvent Bisalt ether-based electrolyte Graphite anode NCM||graphite battery Interfacial optimization

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Atmospheric VOCs in an industrial coking facility and the surrounding area:Characteristics,spatial distribution and source apportionment

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Journal of environmental Sciences 2024年第4期138卷 660-670页

作者： Meicheng Wen Weiqiang Deng Jin Huang Shu Zhang Qinhao Lin ChaoWang Shengtao Ma Wanjun Wang Xin Zhang Guiying Li Taicheng An Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and Health Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlInstitute of Environmental Health and Pollution controlGuangdong University of TechnologyGuangzhou 510006China Guangdong Engineering Technology Research center for Photocatalytic Technology Integration and Equipment Guangzhou Key Laboratory of Environmental Catalysis and Pollution ControlSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China Institute of environmental Science Shanxi UniversityTaiyuan 030006China

Industrial coking facilities are an important emission source for volatile organic compounds(VOCs).This study analyzed the atmospheric VOC characteristics within an industrial coking facility and its surrounding *** concentrations of total VOCs(TVOCs)in the surrounding residential activity areas(R1 and R2),the coking facility(CF)and the control area(CA)were determined to be 138.5,47.8,550.0,and 15.0μg/m^(3),*** cold drum process and coking and quenching areas within the coking facility were identified as the main polluting *** spatial variation in VOCs composition was analyzed,showing that VOCs in the coking facility and surrounding areas were mainly dominated by aromatic compounds such as BTX(benzene,toluene,and xylenes)and naphthalene,with concentrations being negatively correlated with the distance from the coking facility(p<0.01).The sources of VOCs in different functional areas across the monitoring area were analyzed,finding that coking emissions accounted for 73.5%,33.3% and 27.7% of TVOCs in CF,R1 and R2,*** results demonstrated that coking emissions had a significant impact on VOC concentrations in the areas surrounding coking *** study evaluates the spatial variation in exposure to VOCs,providing important information for the influence of VOCs concentration posed by coking facility to surrounding residents and the development of strategies for VOC abatement.

关键词： Coking facility Volatile organic compounds Emission inventory Spatial distribution Source apportionment

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Grapevine-like high entropy oxide composites boost high-performance lithium sulfur batteries as bifunctional interlayers

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Green energy & Environment 2024年第3期9卷 565-572页

作者： Huarong Fan Yubing Si Yiming Zhang Fulong Zhu Xin Wang Yongzhu Fu College of Chemistry and center of Green catalysis Zhengzhou UniversityZhengzhou450001China School of Materials and energy University of Electronic Science and Technology of ChinaChengdu611731China

Lithium-sulfur batteries(LSBs)with high energy densities have been demonstrated the potential for energy-intensive demand ***,their commercial applicability is hampered by hysteretic electrode reaction kinetics and the shuttle effect of lithium polysulfides(LiPSs).In this work,an interlayer consisting of high-entropy metal oxide(Cu_(0.7)Fe_(0.6)Mn_(0.4)Ni_(0.6)Sn_(0.5))O_(4) grown on carbon nanofibers(HEO/CNFs)is designed for *** CNFs with highly porous networks provide transport pathways for Li^(+) and e^(-),as well as a physical sieve effect to limit LiPSs *** particular,the grapevine-like HEO nanoparticles generate metal-sulfur bonds with LiPSs,efficiently anchoring active *** unique structure and function of the interlayer enable the LSBs with superior electrochemical performance,i.e.,the high specific capacity of 1381 mAh g^(-1) at 0.1 C and 561 mAh g^(-1) at 6 *** work presents a facile strategy for exploiting high-performance LSBs.

关键词： Electrospun carbon nanofibers Grapevine-like morphology Hierarchical physical sieve effect High-entropy induced chemisorption Lithium-sulfur battery

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A perspective to ammonia-hydrogen energy industry in China

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Science China Chemistry 2024年第6期67卷 1765-1775页

作者： Baoshun Zhang Wangyang Ji Jiewei Zhu Baian Shen Menghao Lv Bin Zhang Tihu Wang Yifu Yu Department of Chemistry Institute of Molecular PlusSchool of ScienceTianjin UniversityTianjin300072China Tianjin University-Asia Silicon Joint Research center of Ammonia-hydrogen New energy Asia Silicon(Qinghai)Co.Ltd.Xining810007China Department of catalysis Science and Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

1 *** meet the 1.5℃ climate goal in our planet,the world is making a hard work for decarbonization[1-5].Constructing a clean energy system based on green energy is considered as the most promising way to achieve the ... 详细信息

关键词： ammonia planet energy

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Nano-sized stationary phase packings retained by single-particle frit for microchip liquid chromatography

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Chinese Chemical Letters 2024年第4期35卷 486-489页

作者： Wangyan Hu Ke Li Xiangnan Dou Ning Li Xiayan Wang center Excellence for environmental Safety and Biological Effects Beijing Key Laboratory for Green Catalysis and SeparationDepartment of ChemistryBeijing University of TechnologyBeijing 100124China center for environmental Metrology National Institute of MetrologyBeijing 100029China

Modern chromatography is increasingly focused on miniaturization and integration. Compared to conventional liquid chromatography, microfluidic chip liquid chromatography(microchip-LC) has the potential due to its zero-dead volume connection and ease of integration. Nano-sized packings have the potential to significantly enhance separation performance in microchip-LC. However, their application has been hindered by packing difficulties. This study presents a method for packing nano-sized silica particles into a microchannel as the stationary phase. The microchip-LC packed column was prepared by combining the weir and the porous silica single-particle as frit to retain the packing particles. A surface tensionbased single-particle picking technique was established to insert porous single-particle frit into glass microchannels. Additionally, we developed a slurry packing method that utilizes air pressure to inject nano-sized packing into the microchannel. Pressure-driven chromatographic separation was performed using this nano-packed column integrated into a glass microchip. The mixture of four PAHs was successfully separated within just 8 min using a 5 mm separation channel length, achieving high theoretical plates(10~6plates/m). Overall, these findings demonstrate the potential of utilizing nano-sized packings for enhancing chromatographic performance in microchip systems.

关键词： Nano-size packing Single-particle frit Packed column Microchip LC Chromatographic separation

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Atmospheric chemistry of 2-nitrobenzaldehyde:Initiated by photo-excitation,OH-oxidation,and small TiO_(2) clusters adsorption catalysis

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Journal of environmental Sciences 2024年第5期139卷 123-137页

作者： Feng-Yang Bai Xiang-Huan Liu Ting-Ting Meng Zhou Yu Yi-Chen Wang Shuang Ni Zhen Zhao Institute of catalysis for energy and Environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034China

The fate of 2-nitrobenzaldehyde(2-NBA)is of interest in atmospheric chemistry as it is a semi-volatile organic compound with high *** study presents a quantum chemical study of the gas-phase reactions of 2-NBA photo-excitation and OH-oxidation in the absence and presence of small TiO_(2) *** further understand the unknown photolysis mechanism,the photo-reaction pathways of ground singlet state and the lying excited triplet state of 2-NBA were investigated including the initial and subsequent reactions of proton transfer,direct CO,NO_(2),and HCO elimination routes in the presence of O_(2) and ***,the OH-mediated degradation of 2-NBA proceeded via five H-extraction and six OH-addition channels by indirect mechanism,which follows a succession of reaction steps initiated by the formation of weakly stable intermediate *** H-extraction from the-CHO group was the dominant pathway with a negative activation energy of-1.22 kcal/*** calculated rate coefficients at 200–600 K were close to the experimental data in literature within 308-352 K,and the kinetic negative temperature independence was found in both experimental literature and computational ***,2-NBA was favored to be captured onto small TiO_(2) clusters via six adsorption configurations formed via various combination of three types of bonds of Ti…O,Ti…C,and O…H between the molecularly adsorbed 2-NBA and TiO_(2) *** indicted that the chemisorptions of aldehyde oxygen have largest *** results suggested adsorption conformations have a respectable impact on the catalysis *** study is significant for understanding the atmospheric chemistry of 2-nitrobenzaldehyde.

关键词： 2-nitrobenzaldehyde OH radical oxidation Rate coefficient Photolysis mechanism Adsorption catalysis

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