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Pd Pt VO_(x)/CeO_(2)-ZrO_(2):Highly efficient catalysts with good sulfur dioxide-poisoning reversibility for the oxidative removal of ethylbenzene

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Journal of Environmental Sciences 2024年第4期138卷 153-166页

作者： Jia Wang Yuxi Liu Jiguang Deng Lin Jing Xiuqing Hao Xing Zhang Xiaohui Yu Hongxing Dai Beijing Key laboratory for Green catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaLaboratory of Catalysis Chemistry and NanoscienceDepartment of Chemical EngineeringFaculty of Environment and LifeBeijing University of TechnologyBeijing 100124China

The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various techniques.Catalytic activities of these materials in the presence of H_(2)O or SO_(2)were evaluated for the oxidation of ethylbenzene(EB).The PdPtVO_(x)/CZO sample exhibited high catalytic activity,good hydrothermal stability,and reversible sulfur dioxide-poisoning performance,over which the specific reaction rate at 160℃,turnover frequency at 160℃(TOF_(Pd or Pt)),and apparent activation energy were 72.6 mmol/(g_(Pt)·sec)or 124.2 mmol/(g_(Pd)·sec),14.2 sec^(-1)(TOF_(Pt))or 13.1 sec^(-1)(TOF_(Pd)),and 58 k J/mol,respectively.The large EB adsorption capacity,good reducibility,and strong acidity contributed to the good catalytic performance of PdPtVO_(x)/CZO.Catalytic activity of PdPtVO_(x)/CZO decreased when 50 ppm SO_(2)or(1.0 vol.%H_(2)O+50 ppm SO_(2))was added to the feedstock,but was gradually restored to its initial level after the SO_(2)was cut off.The good reversible sulfur dioxide-resistant performance of PdPtVO_(x)/CZO was associated with the facts:(i)the introduction of SO_(2)leads to an increase in surface acidity;(ii)V can adsorb and activate SO_(2),thus accelerating formation of the SO_(x)^(2-)(x=3 or 4)species at the V and CZO sites,weakening the adsorption of sulfur species at the PdPt active sites,and hence protecting the PdPt active sites to be not poisoned by SO_(2).EB oxidation over PdPtVO_(x)/CZO might take place via the route of EB→styrene→phenyl methyl ketone→benzaldehyde→benzoic acid→maleic anhydride→CO_(2)and H_(2)O.

关键词： Ceria-zirconia Supported palladium-platinum-vanadium catalyst Volatile organic compound Ethylbenzene oxidation Sulfur dioxide resistance

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Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li Department of Chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State Key laboratory of Surface Physics and Department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable challenge.Herein,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as templates.The key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon matrix.The mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion lengths.This method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

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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 hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still unclear.Here,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light sources.Xe 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 min.The xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and carbonyls.Among 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 xylenes.Moreover,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 risk.Therefore,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 xylenes.The 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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Mechanisms of isomerization and hydration reactions of typicalβ-diketone at the air-droplet interface

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Journal of Environmental Sciences 2024年第7期141卷 225-234页

作者： Yuemeng Ji Weiyong Luo Qiuju Shi Xiaohui Ma Ziqi Wu Weina Zhang Yanpeng Gao Taicheng An Guangdong-Hong Kong-Macao Joint laboratory for Contaminants Exposure and Health Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlInstitute Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key laboratory of Environmental catalysis and Pollution Control Key Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of EducationSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Acetylacetone(AcAc)is a typical class ofβ-diketones with broad industrial applications due to the property of the keto-enol isomers,but its isomerization and chemical reactions at the air-droplet interface are still unclear.Hence,using combined molecular dynamics and quantum chemistry methods,the heterogeneous chemistry of AcAc at the air-droplet interface was investigated,including the attraction of AcAc isomers by the droplets,the distribution of isomers at the air-droplet interface,and the hydration reactions of isomers at the air-droplet interface.The results reveal that the preferential orientation of two AcAc isomers(keto-and enol-AcAc)to accumulate and accommodate at the acidic air-droplet interface.The isomerization of two AcAc isomers at the acidic air-droplet interface is more favorable than that at the neutral air-droplet interface because the“water bridge”structure is destroyed by H_(3)O^(+),especially for the isomerization from keto-Ac Ac to enol-AcAc.At the acidic air-droplet interface,the carbonyl or hydroxyl O-atoms of two AcAc isomers display an energetical preference to hydration.Keto-diol is the dominant products to accumulate at the air-droplet interface,and excessive keto-diol can enter the droplet interior to engage in the oligomerization.The photooxidation reaction of AcAc will increase the acidity of the air-droplet interface,which indirectly facilitate the uptake and formation of more keto-diol.Our results provide an insight into the heterogeneous chemistry ofβ-diketones and their influence on the environment.

关键词： Acetylacetone Air-droplet interface Theoretical simulation Isomerization Hydration reaction mechanism

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Copper-catalyzed C(sp)-H aryl amination enables modular synthesis of quinolines and 2-quinolinones

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Science China Chemistry 2024年第2期67卷 595-603页

作者： Yang Gao Haixia Li Simin Yang Yanping Huo Qian Chen Xianwei Li Zhe Wang Xiao-Qiang Hu School of Chemical engineering and Light Industry Guangdong University of TechnologyGuangzhou510006China Jieyang Branch of Chemistry and Chemical engineering Guangdong laboratory Jieyang515200China Key laboratory of catalysis and Energy Materials Chemistry of Ministry of Education&Hubei Key laboratory of catalysis and Materials Science School of Chemistry and Materials ScienceSouth-Central University for NationalitiesWuhan430074China

Herein,we disclose a novel copper-catalyzed C(sp)-H aryl amination of terminal alkynes with anthranils,enabling the rapid generation of highly reactive secondary N-aryl ynamines for the modular synthesis of structurally diverse C2-substituted quinolines and 2-quinolinones.The in-situ formed carbonyl-ynamines are prone to tautomerize to carbonyl-ketenimines,which can efficiently react with a series of nucleophiles,including amines,alcohols,phenols,thiols,thiophenols,active-methylene compounds,and even water to produce various quinoline derivatives with the generation of H_(2)O as a sole and green byproduct.This method also unlocks a practical route to create various quinoline-fused heterocycles and can be successfully applied to the late-stage modification of complex molecules and the concise synthesis of bioactive targets.Mechanistic studies reveal a coppercatalyzed inner-sphere nitrene transfer process by using anthranils as novel aryl nitrene precursors.

关键词： copper catalysis anthranils C(sp)-H aryl amination carbonyl-ketenimines quinolines

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Design and construction of size-controlled CoO/CS catalysts for Fischer–Tropsch synthesis

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Nano Research 2024年第4期17卷 2520-2527页

作者： Wei Sun Ting Kuang Guiyou Wei Yue Li Yaqin Liu Shuai Lyu Yuhua Zhang Jinlin Li Li Wang Key laboratory of catalysis and Energy Materials Chemistry of Ministry of Education&Hubei Key laboratory of catalysis and Materials Science South-Central Minzu UniversityWuhan 430074China Hubei Key laboratory of Biomass Fibers and Eco-dyeing&Finishing College of Chemistry and Chemical EngineeringWuhan Textile UniversityWuhan 430200China

The use of supported Co-based catalysts is widespread in various catalytic reactions due to their unique structures.The structural sensitivity of these catalysts is closely linked to their particle size and crystal form.Consequently,comprehending the structure–activity relationship requires the development of well-defined Co-based catalysts.Herein,we employed a colloidal wet chemical process and a heterogeneous nucleation method to prepare well-defined Co-based catalysts supported by inert carbon nanospheres.The nanospheres’surface possesses abundant functional groups that efficiently capture metal complexes and facilitate the nucleation and growth of CoO nanoparticles.By adjusting the Co source concentration,solvent molar ratio,and nucleation growth kinetics,we successfully prepared CoO/carbon sphere(CS)catalysts with different particle sizes and crystal forms.The influence of metallic face-centered cubic(fcc)-Co^(0) particle size in the range of 6.6–17.6 nm on the performance of Fischer–Tropsch synthesis(FTS)using well-defined CoO/CS catalysts has been investigated.The result demonstrated that the turnover frequency(TOF)remained constant for CoO/CS catalysts with metallic fcc-Co^(0) particle size larger than 7.7 nm.However,both the selectivity and the activity changed for CoO/CS catalysts with smaller particles(<7.7 nm).Significantly,when metallic fcc-Co^(0) particle size was reduced from 17.6 to 7.7 nm,the cobalt time yield increased to 6.7μmolCO·gCo^(-1)·s^(-1),indicating improved catalytic activity.At the same time,the CH_(4) selectivity decreased to 4.9%,suggesting a higher preference for hydrocarbon production.These findings demonstrate the importance of particle size in Co catalyzed Fischer–Tropsch synthesis.The use of well-defined CoO/CS catalysts offers valuable insights into the structure–activity relationship,leading to a better understanding of Co catalyzed Fischer–Tropsch synthesis.

关键词： Fischer–Tropsch synthesis(FTS) cobalt size effects phase effects carbon nanospheres

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Uniform lithium deposition induced by copper phthalocyanine additive for durable lithium anode in lithium-sulfur batteries

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Chinese Chemical Letters 2024年第5期35卷 447-452页

作者： Ting Hu Yuxuan Guo Yixuan Meng Ze Zhang Ji Yu Jianxin Cai Zhenyu Yang Key laboratory of Jiangxi Province for Environment and Energy catalysis School of Chemistry and Chemical EngineeringNanchang UniversityNanchang 330031China

Copper phthalocyanine(CuPc)is adopted as an electrolyte additive to stabilize lithium anode for lithiumsulfur(Li-S)batteries.CuPc with a planar molecular structure and lithiophilic N-containing group,is likely to be adsorbed on the surface of Li anode to form a coating layer,which can restrict the direct contact between Li anode and solvents,and guide the uniform deposition of Li^(+)ions.The Li||Li symmetric cells demonstrate a stable cycle performance,and Li||Cu cells show high Coulombic efficiencies.In Li-S batteries,the formed stable solid-electrolyte interface(SEI)film containing copper sulfides can protect Li anode from the polysulfide corrosion and side reactions with the electrolyte,leading to the compact and smooth surface morphology of Li anode.Therefore,the Li-S batteries with CuPc additive deliver much higher capacity,better cycle performance and rate capability as compared to the one without CuPc additive.

关键词： Copper phthalocyanine Electrolyte additive Stable SEI film Stabilized Li anode Lithium-sulfur batteries

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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 environment.Average 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),respectively.The cold drum process and coking and quenching areas within the coking facility were identified as the main polluting processes.The 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,respectively.These results demonstrated that coking emissions had a significant impact on VOC concentrations in the areas surrounding coking facility.This 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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Crystal facet-dependent CO_(2)cycloaddition to epoxides over ZnO catalysts

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Frontiers of Chemical Science and engineering 2024年第5期18卷 49-59页

作者： Yongjian Wei Ying Li Yunfei Xu Yinghui Sun Tong Xu Haiou Liang Jie Bai Inner Mongolia Key laboratory of Industrial catalysis Hohhot 010051China College of Chemical engineering Inner Mongolia University of TechnologyHohhot 010051China

With regard to green chemistry and sustainable development,the fixation of CO_(2)into epoxides to form cyclic carbonates is an attractive and promising pathway for CO_(2)utilization.Metal oxides,renowned as promising eco-friendly catalysts for industrial production,are often undervalued in terms of their impact on the CO_(2)addition reaction.In this work,we successfully developed ZnO nanoplates with(002)surfaces and ZnO nanorods with(100)surfaces via morphology-oriented regulation to explore the effect of crystal faces on CO_(2)cycloaddition.The quantitative data obtained from electron paramagnetic resonance spectroscopy indicated that the concentration of oxygen vacancies on the ZnO nanoplate surfaces was more than twice that on the ZnO nanorod surfaces.Density functional theory calculations suggested that the(002)surfaces have lower adsorption energies for CO_(2)and epichlorohydrin than the(100)surfaces.As a result,the yield of cyclochloropropene carbonate on the ZnO nanoplates(64.7%)was much greater than that on the ZnO nanorods(42.3%).Further evaluation of the reused catalysts revealed that the decrease in the oxygen vacancy concentration was the primary factor contributing to the decrease in catalytic performance.Based on these findings,a possible catalytic mechanism for CO_(2)cycloaddition with epichlorohydrin was proposed.This work provides a new idea for the controllable preparation of high-performance ZnO catalysts for the synthesis of cyclic carbonates from CO_(2)and epoxides.

关键词： carbon dioxide cycloaddition zinc oxide crystal face oxygen vacancy

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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 performance.To address these drawbacks,this study investigated the effect of low intensity ultrasound treatment combined with hydroxylamine(NH2OH)on the performance of partial nitrification.Results 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% NRR.Mechanis-tic analysis showed that NH2OH enhanced ammonia oxidation,inhibited nitrite-oxidizing bacteria(NOB)activity and shortened the time required for partial nitrification initiation.Furthermore,ultrasonication combined with NH2OH dosing stimulated EPS(extracellular polymeric substances)secretion,increased carbonyl,hydroxyl and amine functional group abundances and enhanced mass transfer.In 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 group.Collectively,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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