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Boosting the catalytic performance of Cu-SAPO-34in NO_(x) removal via hydrothermal treatment

Journal of environmental Sciences 2024年第1期135卷 640-655页

作者： Xiaoyan Tian Huimin Wang Siyuan Xu Lianyun Gao Jinyan Cao Jianjun Chen Qiulin Zhang Ping Ning Jiming Hao Faculty of Environmental Science and Engineering Kunming University of Science and TechnologyKunming 650500China National-Regional Engineering Center for Recovery of Waste Gases from Metallurgical and Chemical Industries Kunming University of Science and TechnologyKunming 650500China School of Environment State Key Joint Laboratory of Environment Simulation and Pollution ControlTsinghua UniversityBeijing 100084China

Phosphate ions promoted Cu-SAPO-34(P-Cu-SAPO-34)were prepared using bulk CuO particles as Cu^(2+)precursor by a solid-state ion exchange technique for the selective catalytic reduction of NO_(x) with NH_3(NH_3-SCR).The effects of high temperature(H-T)hydrothermal aging on the NO_(x) removal(de-NO_(x))performance of Cu-SAPO-34 with and without phosphate ions were systematically investigated at atomic *** results displayed that both Cu-SAPO-34 and P-Cu-SAPO-34 presented relatively poor NO_(x) removal activity with a low conversion(<30%)at 250-500℃.However,after H-T hydrothermal treatment(800℃ for 10 hr at 10%H_2O),these two samples showed significantly satisfied NO_(x) elimination performance with a quite high conversion(70%-90%)at 250-500℃.Additionally,phosphate ions decoration can further enhance the catalytic performance of Cu-SAPO-34 after hydrothermal treatment(Cu-SAPO-34H).The textural properties,morphologies,structural feature,acidity,redox characteristic,and surface-active species of the fresh and hydrothermally aged samples were analyzed using various characterization *** systematical characterization results revealed that increases of 28%of the isolated Cu^(2+)active species(Cu^(2+)-2Z,Cu(OH)^(+)-Z)mainly from bulk CuO and 50%of the Bronsted acid sites,the high dispersion of isolated Cu^(2+)active component as well as the Bronsted acid sites were mainly responsible for the accepted catalytic activity of these two hydrothermally aged samples,especially for P-Cu-SAPO-34H.

关键词： NH_(3)-SCR Cu-SAPO-34 Hydrothermal induced Phosphate ions

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Solid Bronsted acidity boosts adsorption reactivity of nano-adsorbent for water decontamination

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Frontiers of environmental Science & Engineering 2024年第7期18卷 23-34页

作者： Sikai Cheng Zhixian Li Kaisheng Zhang Qingrui Zhang Xiaolin Zhang Bingcai Pan State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China Environmental Materials and Pollution Control Laboratory Institute of Solid State PhysicsHFIPSChinese Academy of SciencesHefei 230031China State Key Laboratory of Metastable Materials Science and Technology Yanshan UniversityQinhuangdao 066004China Hebei Key Laboratory of Heavy Metal Deep-remediation in Water and Resource Reused Qinhuangdao 066004China Research Center for Environmental Nanotechnology(ReCENT) Nanjing UniversityNanjing 210023China

Despite the development of various Lewis acidic nano-adsorbents for fluoride removal through innersphere coordination,strong competition for hydroxyl ions still hinders efficient water *** addition,the critical issue of polysilicate scaling that results from the ubiquitous silicates must be *** tackle these issues,an alternative approach to enhancing adsorption reactivity by modifying nano-adsorbents with dual Lewis and Bronsted acidity is *** feasibility of this approach is demonstrated by growing zirconium phosphate(ZrP)inside a gel-type anion exchanger,N201,to produce nanocomposite ZrP@N201,in which the confined ZrP contained an otherwise metastable amorphous phase with Lewis acidic Zr^(4+) sites and Bronsted acidic monohydrogen phosphate groups(-O_(3)POH).Compared with the Lewis acidic nano-zirconium oxide analog(HZ0@N201),ZrP@N201 exhibited a greatly improved adsorption capacity(117.9 vs.52.3 mg/g-Zr)and mass transfer rate(3.56×10^(-6) vs.4.55×10^(-7) cm/s),while bulk ZrP produced a thermodynamically stableα-phase with Bronsted acidity that exhibited negligible adsorption capability toward *** enhanced defluoridation activity of ZrP@N201 is attributed to Bronsted acidity and the increased outer electron density of ZA+sites,as corroborated using XPS and solid-state NMR ***,Bronsted acidity strengthens the resistance of ZrP@N201 to silicate,allowing its full regeneration during cyclic *** tests demonstrated 3-10 times the amount of clean water from(waste)for ZrP@N201 as compared to both HZO@N201 and the widely used activated aluminum *** study highlights the potential of developing nano-adsorbents with dual acidities for various environmental remediation applications.

关键词： Nanocomposite Selective adsorption Fluoride removal Dual Lewis and Bronsted acidity Regeneration

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Coking of Pt/γ-Al_(2)O_(3) catalyst in landfill gas deoxygen and its effects on catalytic performance

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Chinese Journal of Chemical Engineering 2023年第5期57卷 224-232页

作者： Xinyu Yang Zezhi Chen Huijuan Gong State Key Laboratory of Pollution Control and Resource Reuse School of EnvironmentNanjing UniversityNanjing 210023China Center of Materials Analysis Nanjing UniversityNanjing 210093China

Catalytic oxidation of CH_(4) has been proved to be an attractive option for landfill gas(LFG) ***, coking of catalysts in catalytic LFG deoxygen has been clearly observed in industrial applications. In this regard, it is necessary to investigate whether coke deposition originates from CH_(4) or volatile organic compounds present in LFG, and the influence of coke deposition on catalytic performance. Herein,we evaluate the LFG deoxygen on Pt/γ-Al_(2)O_(3) catalyst in simulated LFG(CH_(4), CO_(2), O_(2), N_(2)) and its co-feed with representative volatile organic compounds, ethylbenzene, toluene, benzene and cyclohexane. The results show that the coking of the catalyst is originated from volatile organic compounds rather than CH_(4). The Pt/γ-Al_(2)O_(3) catalyst does not deactivate during LFG deoxygen process, even significant amount of coke deposited, up to 18.15%(mass). Characterization analyses reveal that although coke deposition overall covers the catalyst surface, resulting in mesopores blockage and a reduced number of accessible Pt sites, however, the coke formed, H-rich carbonaceous components, behaves as counterpart for O_(2) elimination. Besides, the coke deposited is mainly filamentous. Thus, coke formation has little negative effect on the overall catalytic performance of Pt/γ-Al_(2)O_(3) catalyst ultimately. The results obtained in this work are helpful for the rational design of robust Pt based catalysts for LFG deoxygen without undue attention to their coking properties, and also favor the innovation of more attractive purification scheme configurations.

关键词： Landfill gas Deoxygen Pt/γ-Al_(2)O_(3) Volatile organic compounds Coke deposition

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Acetylacetone effectively controlled the secondary metabolites of Microcystis aeruginosa under simulated sunlight irradiation

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Journal of environmental Sciences 2024年第1期135卷 285-295页

作者： Xiaomeng Wang Yixin Luo Shujuan Zhang Lixiang Zhou Department of Environmental Engineering College of Resources and Environmental SciencesNanjing Agricultural UniversityNanjing 210095China The State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China

Inactivation of cyanobacterial cells and simultaneous control of secondary metabolites is of significant necessity for the treatment of cyanobacteria-laden ***(AcAc)has been reported a specific algicide to inactivate Microcystis aeruginosa(***)and an effective light activator to degrade *** study systematically investigated the photodegradation ability of AcAc under xenon(Xe)irradiation on the secondary metabolites of ***,mainly algal organic matter(AOM),especially toxic microcystin-LR(MC-LR).Results showed that AcAc outperformed H_(2)O_(2)in destructing the protein-like substances,humic acid-like matters,aromatic proteins and fulvic-like substances of *** MC-LR(250μg/L),0.05 mmol/L AcAc attained the same degradation efficiency(87.0%)as 0.1mmol/L H_(2)O_(2).The degradation mechanism of Xe/AcAc might involve photo-induced energy/electron transfer and formation of carbon center *** conditions(pH>9.0)were detrimental to the photoactivity of AcAc,corresponding to the observed degradation rate constant(k_(1)value)of MC-LR drastically decreasing to 0.0013 min^(-1)as solution pH exceeded *** PO_(4)^(3-)and HCO_(3)^(-)ions had obvious inhibition effects,whereas NO_(3)^(-)slightly improved k_(1)value from 0.0277 min^(-1)to 0.0321 min^(-1).The presence of AOM did not significantly inhibit MC-LR degradation in Xe/AcAc *** addition,the biological toxicity of MC-LR was greatly reduced after *** results demonstrated that AcAc was an alternative algicidal agent to effectively inactivate algal cells and simultaneously control the secondary metabolites after cell ***,the concentration and irradiation conditions should be further optimized in practical application.

关键词： Microcystis aeruginosa Photodegradation Acetylacetone Secondary metabolites Microcystin

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Seasonal variations of microbial community and antibiotic resistome in a suburb drinking water distribution system in a northern Chinese city

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Journal of environmental Sciences 2023年第5期127卷 714-725页

作者： Yanchu Ke Wenjun Sun Zibo Jing Zhinan Zhao Shuguang Xie State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China School of Environment Tsinghua UniversityBeijing 100084China Research Institute for Environmental Innovation(Suzhou)Tsinghua Suzhou 215163China

Antibiotic resistance genes(ARGs)are an emerging issue for drinkingwater ***,the seasonal variation of ARGs in drinking water distribution systems(DWDS)is still *** work revealed the tempo-spatial changes of microbial community,ARGs,mobile genetic elements(MGEs)co-occurring with ARGs,ARG hosts in DWDS bulk water by means of metagenome *** microbial community and antibiotic resistome varied with sampling season and ***,ammonia,chlorite and total plate count(TPC)drove the variations of microbial community ***,environmental parameters(total organic carbon(TOC),chlorite,TPC and hardness)shifted antibiotic *** and MGEs co-occurring with ARGs showed higher relative abundance in summer and autumn,which might be attributed to detached pipe *** particular,ARG-bacitracin and plasmid were the predominant ARG and MGE,*** hosts changed with season and site and were more diverse in summer and *** winter and spring,Limnohabitans and Mycobacterium were the major ARG hosts as well as the dominant genera in microbial *** addition,in summer and autumn,high relative abundance of Achromobacter and Stenotrophomonas were the hosts harboring many kinds of ARGs and MGEs at site in a residential zone(0.4 km from the water treatment plant).Compared with MGEs,microbial community had a greater contribution to the variation of antibiotic *** work gives new insights into the dynamics of ARGs in full-scale DWDS and the underlying factors.

关键词： Drinking water distribution system Seasonal change Microbial community Antibiotic resistance genes Mobile genetic elements

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Insights into effects of algae on decay and distribution of bacterial pathogens in recreational water:Implications for microbial risk management

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Journal of environmental Sciences 2022年第3期34卷 92-103页

作者： Tingting Fang Zuotao Zhang Hui Wang Matt Rogers Qijia Cui State Key Joint Laboratory on Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Department of Civil and Environmental Engineering National University of SingaporeEngineering Drive 3117576Singapore

The decay and distribution of bacterial pathogens in water is an important information for the health risk assessment to guide water safety management, and suspended algae might affect bacterial pathogens in water. This study established microcosms to investigate the effects of algae-related factors on the representative indicators and opportunistic pathogen species in water. We found that suspended algae increased the persistence of targeted species by 1-2 orders of magnitude of concentrations compared to microcosms without algae;and the effect of algae on microbial survival was affected by water nutrient levels(i.e., carbon, nitrogen and phosphorus), as the increased microbial persistence were correlated to the increased algae concentrations with more nutrient supplies. Moreover, decay and distribution profiles of representative species were determined. The three opportunistic pathogen species( Pseudomonas aeruginosa, Aeromonas hydrophila and Staphylococcus aureus) showed lower decay rates(0.82–0.98/day, 0.76–0.98/day, 0.63–0.87/day) largely affected by algae-related factors, while the enteric species( Escherichia coli and Enterococcus faecalis) had higher decay rates(0.94–1.31/day, 0.89–1.21/day) with little association with algae, indicating the propensity for attachment to algae is an important parameter in microbial fate. Together results suggest suspended algae played an evident role in the decay and distribution of bacterial pathogens, providing important implications regarding microbial safety in recreational water.

关键词： Suspended algae Bacterial pathogen decay Bacterial pathogen distribution Recreational water Microbial risk assessment

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"Forever chemicals":a sticky environmental problem

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Frontiers of environmental Science & Engineering 2024年第10期18卷 175-183页

作者： Junhua Fang Shaolin Li Rongliang Qiu Wei-Xian Zhang College of Environmental Science and Engineering State Key Laboratory of Pollution Control and Resource ReuseTongji UniversityShanghai 200092China Guangdong Laboratory for Lingnan Modern Agriculture Guangzhou 510642China College of Natural Resources and Environment Guangdong Provincial Key Laboratory of Agricultural&Rural Pollution Abatement and Environmental SafetySouth China Agricultural UniversityGuangzhou 510642China

The discovery and widespread use of per-and poly-fluoroalkyl substances(PFAS)have exemplified the beneficial role of chemistry in modern life,yet *** also underscored significant environmental and health *** "forever chemicals"due to their remarkable persistence,PFAS present formidable challenges in terms of contamination and *** to address these challenges have led to the development of innovative degradation technologies,such as hydrothermal alkali treatment(HALT),low-temperature mineralization,and mechanochemical degradation,offering promising solutions to PFAS ***,these advancements must be accompanied by robust investment in research,collaboration among stakeholders,and global responsibility to ensure effective management of PFAs contamination and mitigate its adverse impacts on ecosystems and humanhealth.

关键词： PFAS Degradation technologies environmental remediation Global responsibility

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Mechanism for the promotional formation of NH_(4)^(+) by SO_(2) on different mineral dust surfaces

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Particuology 2023年第4期75卷 109-118页

作者： Hao Li Qingxin Ma Biwu Chu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-environmental SciencesChinese Academy of SciencesBeijing100085China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen361021China Institute of Atmospheric Physics Chinese Academy of SciencesBeijing100029China

Ammonium is an important atmospheric particulate component that dictates many environmental *** promotion of the heterogeneous conversion of NH_(3) to NH_(4)^(+) by SO_(2) on different mineral dust surfaces displays remarkable discrepancies,especially on MgO and α-Fe2O3 surfaces,however,the underlying mechanisms are not well ***,using periodic density functional theory(DFT)calculation and Born-Oppenheimer molecular dynamics(BOMD)simulation,we explored the hetero-geneous adsorption of NH_(3) on MgO(110)and α--Fe2O3(001)surfaces in the presence and absence of SO_(2).The results show that on MgO(110)surface,hydrogen-bonding interactions of NH_(3) on both adsorbed hydroxyl or bisulfite/bisulfate sites are observed no matter whether SO_(2) is present or ***,on theα-Fe2O3(001)surface,significant conversion of NH_(3) to NH_(4)^(+)occurs with the coexistence of SO_(2),which is due to the hydrogen transfer reaction from surface HSO4 to N in NH_(3).The fundamental reason may be that the stronger electron affinity of Fe3+than Mg2+results in adsorbed bisulfate and/or bisulfite with greater acidity on α-Fe2O3 surface than MgO *** results give a molecular-level explanation for the heterogeneous conversion of NH_(3) to NH_(4)^(+)on different mineral dust surfaces under complex air pollution *** the fact that ammonium is abundant in secondary particulates,this work would help in understanding the rapid conversion of ammonia to ammonium and in developing classification governance policies for the key precursor pollutants in China.

关键词： Mineral dust Heterogeneous reaction Theoretical calculation Ammonium SO_(2)

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Synergically regulated silver species and surface oxygen on manganese oxide for promoted activity of formaldehyde oxidation

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Journal of environmental Sciences 2024年第4期138卷 709-718页

作者： Shuo Hu Jianghao Zhang Xueyan Chen Xiaoxiao Qin Jinshui Yao Changbin Zhang School of Materials Science&Engineering Qilu University of Technology(Shandong Academy of Sciences)Jinan 250353China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China

Formaldehyde(HCHO)is a common indoor pollutant that is detrimental to human *** efficient removal has become an urgent demand to reduce the public health *** this work,Ag-MnO_(x)-based catalysts were prepared and activated under different atmosphere(i.e.,air,hydrogen(H_(2))and carbon monoxide(CO))for efficient oxidation of *** catalyst activated with CO(Ag/Mn-CO)displayed the highest activity among the tested samples with 90% conversion at 100℃ under a gas space velocity of 75,000 mL/(g_(cat)·hr).Complementary characterizations demonstrate that CO reduction treatment resulted in synergically regulated content of surface oxygen on support to adsorb/activate HCHO and size of Ag particle to dissociate oxygen to oxidize the adsorbed *** contrast,other catalysts lack for either abundant surface oxygen species or metallic silver with the appropriate particle size,so that the integrate activity is limited by one specific reaction *** study contributes to elucidating the mechanisms regulating the oxidation activity of Ag-based catalysts.

关键词： HCHO oxidation Ag-MnO_(x)-based catalyst Activation condition Synergic regulation Surface oxygen Oxidized Ag

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Insight into the effects of C_(3)H_(6)on fresh and hydrothermally aged Cu-SSZ-39 catalysts

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Chinese Chemical Letters 2025年第3期36卷 164-169页

作者： Jinpeng Du Junlin Chen Yulong Shan Tongliang Zhang Yu Sun Zhongqi Liu Xiaoyan Shi Wenpo Shan Yunbo Yu Hong He State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341119China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

Hydrocarbons(HCs),as major poisoning substances,have a crucial influence on NH_(3)-SCR *** this work,the effects of C_(3)H_(6)on fresh and hydrothermally aged Cu-SSZ-39 catalysts with different copper contents were *** catalysts suffered a deactivation above 250℃,especially between 300-400℃,which was mainly related to the reaction between NH_(3)and C_(3)H_(6).However,the hydrothermally aged and the high-copper-loaded Cu-SSZ-39 catalysts could achieve a recovery of NH_(3)-SCR performance at high *** activity recovery was attributed to the oxidation of C_(3)H_(6)by CuxOy species,which therefore inhibited the reaction between NH_(3)and C_(3)H_(6).As a result,more NH_(3)could be available for the NH_(3)-SCR reaction and the Cu-SSZ-39 catalysts could maintain a good catalytic *** on these findings,we proposed that high loaded Cu-SSZ-39 catalysts with a little CuOx formed are preferred for application.

关键词： Diesel vehicle emission NO_(x)abatement NH3-SCR Cu-SSZ-39 zeolite C_(3)H_(6)poisoning

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