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Low-temperature NH_(3) abatement via selective oxidation over a supported copper catalyst with high Cu^(+) abundance

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Journal of environmental Sciences 2024年第9期143卷 12-22页

作者： Zhiming Yang Lin Peng Leneng Yang Mingli Fu Daiqi Ye Peirong Chen guangdong provincial key Laboratory of atmospheric environment and pollution control National Engineering Laboratory for VOCs Pollution Control Technology and EquipmentSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510006China guangdong Chengyi environmental Technology Corp. Shaoguan 512158China

Selective catalytic NH_(3)-to-N_(2) oxidation(NH_(3)-SCO)is highly promising for abating NH_(3) emissions slipped from stationary flue gas after-treatment *** practical application,however,is limited by the non-availability of low-cost catalysts with high activity and N_(2) ***,using defect-rich nitrogen-doped carbon nanotubes(NCNT-AW)as the support,we developed a highly active and durable copper-based NH_(3)-SCO catalyst with a high abundance of cuprous(Cu^(+))*** obtained Cu/NCNT-AW catalyst demonstrated outstanding activity with a T_(50)(*** temperature to reach 50% NH_(3) conversion)of 174℃ in the NH_(3)-SCO reaction,which outperformed not only the Cu catalyst supported on N-free O-functionalized CNTs(OCNTs)or NCNT with less surface defects,but also those most active Cu catalysts in open *** kinetics measurements and temperature-programmed surface reactions using NH_(3)as a probe molecule revealed that the NH_(3)-SCO reaction on Cu/NCNT-AW follows an internal selective catalytic reaction(i-SCR)route involving nitric oxide(NO)as a key *** to mechanistic investigations by X-ray photoelectron spectroscopy,Raman spectroscopy,and X-ray absorption spectroscopy,the superior NH_(3)-SCO performance of Cu/NCNT-AW originated from a synergy of surface defects and ***,surface defects promoted the anchoring of Cu O nanoparticles on N-containing sites and,thereby,enabled efficient electron transfer from N to Cu O,increasing significantly the fraction of SCR-active Cu^(+)sites in the *** study puts forward a new idea for manipulating and utilizing the interplay of defects and N-dopants on carbon surfaces to fabricate Cu^(+)-rich Cu catalysts for efficient abatement of slip NH_(3)emissions via selective oxidation.

关键词： NH_(3)-SCO XANES Localized etching N-doping N_(2) selectivity i-SCR

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One-pot synthesis of N-doped petroleum coke-based microporous carbon for high-performance CO_(2) adsorption and supercapacitors

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Journal of environmental Sciences 2024年第5期139卷 93-104页

作者： Wenfu Zhu Yuqin Wang Fan Yao Xiaohong Wang Haoming Zheng Guangzheng Ye Hairong Cheng Junliang Wu Haomin Huang Daiqi Ye School of environment and Energy South China University of TechnologyGuangzhou 510006China National Engineering Laboratory for VOCs pollution control Technology and Equipment Guangzhou 510006China guangdong provincial key Laboratory of atmospheric environment and pollution control(SCUT) Guangzhou 510006China guangdong provincial Engineering and Technology Research Centre for environmental Risk Prevention and Emergency Disposal South China University of TechnologyGuangzhou 510006China

Waste resource utilization of petroleum coke is crucial for achieving global carbon emission ***,a series of N-doped microporous carbons were fabricated from petroleum coke using a one-pot synthesis *** as-prepared samples had a large specific surface area(up to 2512 m^(2)/g),a moderate-high N content(up to 4.82 at.%),and high population(55%)of ultra-micropores(<0.7 nm).Regulating the N content and ultra-microporosity led to efficient CO_(2)adsorption and *** ambient pressure,the optimal N-doped petroleum coke-based microporous carbon exhibited the highest CO_(2)uptake of 4.25 mmol/g at 25℃ and 6.57 mmol/g at 0℃.These values are comparable or even better than those of numerous previously reported adsorbents prepared by multistep synthesis,primarily due to the existence of *** sample exhibited excellent CO_(2)/N_(2)selectivity at 25℃ owing to the abundant basic pyridinic and pyrrolic N species;and showed superior CO_(2)adsorption-desorption cycling performance,which was maintained at 97% after 10 cycles at 25℃.Moreover,petroleum coke-based microporous carbon,with a considerably high specific surface area and hierarchical pore structure,exhibited excellent electrochemical performance over the N-doped sample,maintaining a favorable specific capacitance of 233.25F/g at 0.5 A/g in 6 mol/L KOH aqueous *** study provides insight into the influence of N-doping on the porous properties of petroleum coke-based ***,the as-prepared carbons were found to be promising adsorbents for CO_(2)adsorption,CO_(2)/N_(2)separation and electrochemical application.

关键词： One-pot synthesis N-doped microporous carbon CO_(2)adsorption CO_(2)/N_(2)selectivity Electrochemical performance

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Recycling of waste aluminum scraps to fabricate sulfidated zero-valent iron-aluminum particles for enhanced chromate removal

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Journal of environmental Sciences 2024年第4期138卷 650-659页

作者： Yahui Zhang Liguo Zhang Jiajia Zeng Shuqun Xu Jianyu Pan Wenzhuo Huang Jianliang Sun Feng Jiang guangdong provincial key Laboratory of Chemical pollution and environmental Safety&MOE key Laboratory of Theoretical Chemistry of environment School of EnvironmentSouth China Normal UniversityGuangzhou 510006China guangdong provincial key Lab of environmental pollution control and Remediation Technology School of Environmental Science&EngineeringSun Yat-Sen UniversityGuangzhou 510275China

Massive waste aluminum scraps produced from the spent aluminum products have high electron capacity and can be recycled as an attractive alternative to materials based on zerovalent iron(Fe^(0))for the removal of oxidative contaminants from *** study thus proposed an approach to fabricate micron-sized sulfidated zero-valent iron-aluminum particles(S-Al^(0)@Fe^(0))with high reactivity,electron selectivity and capacity using recycled waste aluminum scraps.S-Al^(0)@Fe^(0)with a three-layer structure contained zero-valent aluminum(Al^(0))core,Fe^(0) middle layer and iron sulfide(FeS)*** rates of chromate(Cr(Ⅵ))removal by S-Al^(0)@Fe^(0)at pH 5.0-9.0 were 1.6-5.9 times greater than that by sulfidated zero-valent iron(S-Fe^(0)).The Cr(Ⅵ)removal capacity of S-Al^(0)@Fe^(0)was 8.2-,11.3-and 46.9-fold greater than those of S-Fe0,zero-valent iron-aluminum(Al^(0)-Fe^(0))and Fe^(0),*** chemical cost of S-Al^(0)@Fe^(0) for the equivalent Cr(Ⅵ)removal was 78.5%lower than that of S-Fe^(0).Negligible release of soluble aluminum during the Cr(Ⅵ)removal was *** significant enhancement in the reactivity and capacity of S-Al^(0)@Fe^(0)was partially ascribed to the higher reactivity and electron density of the Al0core than Fe^(0).More importantly,S-Al^(0)@Fe^(0) served as an electric cell to harness the persistent and selective electron transfer from the Al^(0)-Fe^(0) core to Cr(Ⅵ)at the surface via coupling Fe^(0)-Fe^(2+)-Fe^(3+)redox cycles,resulting in a higher electron utilization ***,S-Al^(0)@Fe^(0) fabricated using recycled waste aluminum scraps can be a cost-effective and environmentally-friendly alternative to S-Fe^(0) for the enhanced removal of oxidative contaminants in industrial wastewater.

关键词： Recycled waste aluminum scraps Oxidative contaminants Cr(Ⅵ)reduction Sulfidated Al^(0)@Fe^(0)particle Electron transfer

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Performance and mechanism of CO_(2) absorption during the simultaneous removal of SO_(2) and NO_(x) by wet scrubbing process

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Journal of environmental Sciences 2024年第1期135卷 534-545页

作者： Peng Lu Xianhui Yan Lyumeng Ye Dingsheng Chen Dongyao Chen Jianhang Huang Chaoping Cen guangdong Province Engineering Laboratory for Air pollution control South China Institute of Environmental SciencesMinistry of Ecology and EnvironmentGuangzhou 510655China guangdong provincial key Laboratory of Water and Air pollution control Guangzhou 510655China School of environmental Science and Engineering Sun Yat-sen UniversityGuangzhou 510275China

The co-removal of CO_(2)while removing SO_(2)and NOxfrom industrial flue gas has great potential of carbon emission reduction but related research is *** this study,a wet scrubbing process with various urea solutions for desulfurization and denitrification was explored for the possibility of CO_(2)*** results showed that the urea-additive solutions were efficient for NOxand SO_(2)abatement,but deliveredcontrolled by chemical reaction in early stage,then by ash layer diffusion in later stage.

关键词： CO_(2)absorption Synergistic desulfurization and denitrification Wet scrubbing process Urea-NaClO_(2)-Ca(OH)_(2)absorbent Carbonation reaction

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Efficient NO_x abatement by passive adsorption over a Pd-SAPO-34 catalyst prepared by solid-state ion exchange

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Chinese Chemical Letters 2024年第4期35卷 210-213页

作者： Linhui Liu Wuwan Xiong Mingli Fu Junliang Wu Zhenguo Li Daiqi Ye Peirong Chen National Engineering Laboratory for VOCs pollution control Technology and Equipment Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution ControlSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510006China National Engineering Laboratory for Mobile Source Emission control Technology China Automotive Technology&Research Center Co.Ltd.Tianjin 300300China

Palladium-exchanged chabazite(Pd-CHA) zeolites as passive NO_x adsorbers(PNAs) enable efficient purification of nitrogen oxides(NO_x) in cold-start diesel exhausts. Their commercial application, however,is limited by the lack of facile preparation method. Here, high-performance CHA-type Pd-SAPO-34 zeolite was synthesized by a modified solid-state ion exchange(SSIE) method using PdO as Pd precursor,and demonstrated superior PNA performance as compared to Pd-SAPO-34 prepared by conventional wetchemistry strategies. Structural characterization using Raman spectroscopy and X-ray diffraction revealed that the SSIE method avoided water-induced damage to the zeolite framework during Pd loading. Mechanistic investigations on the SSIE process by in situ infrared spectroscopy and X-ray photoelectron spectroscopy disclosed that, while PdO precursor was mainly converted to Pd^(2+) cations coordinated to the zeolite framework by consuming the-OH groups of the zeolite, a portion of PdO could also undergo thermal decomposition to form highly dispersed Pd~0 clusters in the pore channels. This simplified and scalable SSIE method paves a new way for the cost-effective synthesis of defect-free high-performance Pd-SAPO-34 zeolites as PNA catalysts.

关键词： Pd-SAPO-34 Passive NO_x adsorber Pd loading Solid-state ion exchange Pd transformation

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Insights into the mechanism of multiple Cu-doped Co Fe_(2)O_(4)nanocatalyst activated peroxymonosulfate for efficient degradation of Rhodamine B

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Journal of environmental Sciences 2024年第3期137卷 382-394页

作者： Yuanmin Mo Xiaoping Zhang School of environment&Energy South China University of TechnologyGuangzhou Higher Education Mega CentreGuangzhou 510006China The key Laboratory of pollution control and Ecosystem Restoration in Industry Clusters of Ministry of Education Guangzhou 510006China guangdong provincial key Laboratory of Solid Wastes pollution control and Recycling Guangzhou 510006China guangdong provincial Engineering and Technology Research Center for environmental Risk Prevention and Emergency Disposal Guangzhou 510006China

The multiple metal catalyst as a promising nanomaterial has shown excellent activity in the peroxymonosulfate(PMS)activation for pollutant ***,the role of special sites and in-depth understanding of the PMS activation mechanism are not fully *** this study,a Cu-doped CoFe_(2)O_(4)nanocatalyst(0.5CCF)was synthesized by a sol-gel and calcination method,and used for PMS activation to remove Rhodamine B(RhB).The results showed that the Cu doping obviously enhanced the catalytic performance of CoFe_(2)O_(4),with 99.70%of RhB removed by 0.5CCF while 74.91%in the CoFe_(2)O_(4)within 15 *** on the X-ray photoelectron spectroscopy and electrochemical analysis,this could be ascribed to the more low valence of Co and Fe species generated on the 0.5CCF and faster electron transfers occurred in the 0.5CCF due to the Cu *** addition,Cu doping could provide more reaction sites for the 0.5CCF to activate PMS for RhB *** metal species and the surface hydroxyl were the reaction sites of PMS activation,and the surface hydroxyl played an important role in surface-bound reactive species *** the PMS activation,the Cu not only activated PMS to produce reactive oxygen species(ROS),but also regenerated Co^(2+)and Fe^(2+)to accelerate the PMS *** non-radical of ^(1)O_(2)was the main ROS with a 99.35%of contribution rate,and the SO_(5)^(·–)self-reaction was its major *** study provides a new insight to enhance the PMS activation performance of multiple metal catalysts by Cu doping in wastewater treatment.

关键词： Cu-doped CoFe_(2)O_(4)nanocatalyst PMS activation Mechanism Rhodamine B removal

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Aqueous-phase formation of N-containing secondary organic compounds affected by the ionic strength

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Journal of environmental Sciences 2024年第4期138卷 88-101页

作者： Yuqi Gan Xiaohui Lu Shaodong Chen Xinghua Jiang Shanye Yang Xiewen Ma Mei Li Fan Yang Yewen Shi Xiaofei Wang Shanghai key Laboratory of atmospheric Particle pollution and Prevention Department of Environmental Science and EngineeringFudan UniversityShanghai 200433China Shanghai Institute of pollution control and Ecological Security Shanghai 200092China guangdong provincial Observation and Research Station for Coastal Atmosphere and Climate of the Great Bay Area Southern University of Science and TechnologyShenzhen 518055China Institute of Mass Spectrometry and atmospheric environment Guangdong Provincial Engineering Research Center for On-line Source Apportionment System of Air PollutionJinan UniversityGuangzhouChina environmental Monitoring Station of Pudong New District Shanghai 201200China Shanghai Municipal Center for Disease control&Prevention Shanghai 200336China

The reaction of carbonyl-to-imine/hemiaminal conversion in the atmospheric aqueous phase is a critical pathway to produce the light-absorbing N-containing secondary organic compounds(SOC).The formation mechanism of these compounds has been wildly investigated in bulk solutions with a low ionic ***,the ionic strength in the aqueous phase of the polluted atmosphere may be *** is still unclear whether and to what extent the inorganic ions can affect the SOC *** we prepared the bulk solution with certain ionic strength,in which glyoxal and ammonium were mixed to mimic the aqueous-phase *** characterization by High-resolution Mass Spectrometry was performed to identify the N-containing products,and the light absorption of the mixtures was measured by ultraviolet-visible ***-nine N-containing compounds were identified and divided into four categories(N-heterocyclic chromophores,high-molecular-weight compounds with N-heterocycle,aliphatic imines/hemiaminals,and the unclassified).It was observed that the longer reaction time and higher ionic strength led to the formation of more N-heterocyclic chromophores and the increasing of the lightabsorbance of the *** added inorganic ions were proposed to make the aqueous phase somewhat viscous so that the molecules were prone to undergo consecutive and intramolecular reactions to form the *** general,this study revealed that the enhanced ionic strength and prolonged reaction time had the promotion effect on the lightabsorbing SOC *** implies that the aldehyde-derived aqueous-phase SOC would contribute more light-absorbing particulate matter in the industrial or populated area where inorganic ions are abundant.

关键词： Ionic strength Carbonyl-to-imine/hemiaminal Heterocyclic Brown carbon Mass spectrometry Aqueous-phase reaction

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Iodine enrichment in the groundwater in South China and its hydrogeochemical control

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Journal of environmental Sciences 2024年第8期142卷 226-235页

作者： Fengping Zhou Qianting Xu Yuyun Chen Weihua Zhang Rongliang Qiu guangdong provincial key Laboratory of environmental pollution and Remediation Technology Guangdong Provincial Engineering Research Center for Heavy Metal Contaminated Soil RemediationSchool of Environmental Science and EngineeringSun Yat-sen UniversityGuangzhou 510275China Shenzhen Research Institute Sun Yat-sen UniversityShenzhen 518057China guangdong provincial key Laboratory of Agricultural&Rural pollution Abatement and environmental Safety School of Natural Resources and EnvironmentSouth China Agricultural UniversityGuangzhou 510642China guangdong Laboratory for Lingnan Modern Agriculture Guangzhou 510642China

In North China,iodine-rich groundwater has been extensively studied,but few in South *** study aimed to investigate the characteristics of iodine-rich groundwater in South China and identify potential contamination *** results revealed that the average concentration of iodine in groundwater was 890μg/L,with a maximumconcentration of 6350μg/L,exceeding the permitted levels recommended by the World Health Organization(5–300μg/L).Notably,the enrichment of iodide occurred in acidic conditions(pH=6.6)and a relatively low Eh environment(Eh=198.4 mV).Pearson correlation and cluster analyses suggested that the enrichment of iodide could be attributed to the intensified redox process involving Mn(II),iodine(I_(2)),or iodate(IO_(3)^(−))in the *** strong affinity between Mn(II)and I_(2)/IO_(3)^(−)facilitated their interaction,resulting in the formation and mobilization of I^(−)from the soil to the *** experiments further confirmed that reducing substances(such as sodium sulfides,ascorbic acids,and fulvic acids)in the soil with low dissolved oxygen(DO)levels(3.8 mg/L)promoted the oxidation of I^(−)into I_(2)or IO_(3)^(−),leading to its *** research provides new insights into the characteristics and mechanisms of I^(−)enrichment in groundwater in South China,and emphasizes the significance of the redox reactions involving Mn(II)and I_(2)/IO_(3)^(−),as well as the influence of soil properties in regulating the occurrence and transportation of iodine species within groundwater systems.

关键词： Iodine enrichment Acid environment Groundwater South China Manganese

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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 ***,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 *** results reveal that the preferential orientation of two AcAc isomers(keto-and enol-AcAc)to accumulate and accommodate at the acidic air-droplet *** 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 *** the acidic air-droplet interface,the carbonyl or hydroxyl O-atoms of two AcAc isomers display an energetical preference to ***-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 *** photooxidation reaction of AcAc will increase the acidity of the air-droplet interface,which indirectly facilitate the uptake and formation of more *** 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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Transcriptomics and physiological analyses reveal that sulfur alleviates mercury toxicity in rice(Oryza sativa L.)

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Journal of environmental Sciences 2024年第1期135卷 10-25页

作者： Yingmei Huang Jicai Yi Xiaomin Li Fangbai Li National-Regional Joint Engineering Research Center for Soil pollution control and Remediation in South China Guangdong Key Laboratory of Integrated Agro-Environmental Pollution Control and ManagementInstitute of Eco-Environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China Guangzhou Institute of Geochemistry Chinese Academy of SciencesGuangzhou 510640China University of Chinese Academy of Sciences Beijing 100049China College of Life Sciences South China Agricultural UniversityGuangzhou 510642China SCNU environmental Research Institute Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety&MOE Key Laboratory of Theoretical Chemistry of EnvironmentSouth China Normal UniversityGuangzhou 510006China

Mercury(Hg)is one of the most dangerous contaminants and has sparked global concern since it poses a health risk to humans when consumed through ***(S)is a crucial component for plant growth,and S may reduce Hg accumulation in rice ***,the detailed effects of S and the mechanisms underlying S-mediated responses in Hg-stressed rice plants remain ***,to investigate the effects of S addition on rice growth,Hg accumulation,physiological indexes,and gene expression profiles,rice seedlings were hydroponically treated with Hg(20μmol/L Hg Cl_(2))and Hg plus elemental sulfur(100 mg/L).S application significantly reduced Hg accumulation in Hg-stressed rice roots and alleviated the inhibitory effects of Hg on rice growth.S addition significantly reduced Hg-induced reactive oxygen species generation,membrane lipid peroxidation levels,and activities of antioxidant enzymes while increasing glutathione content in *** analysis of roots identified 3,411,2,730,and 581 differentially expressed genes in the control(CK)***,CK ***+S,and Hg ***+S datasets,*** pathway of S-mediated biological metabolism fell into six groups:biosynthesis and metabolism,expression regulation,transport,stimulus response,oxidation reduction,and cell wall *** majority of biological process-related genes were upregulated under Hg stress compared with CK treatment,but downregulated in the Hg+S *** results provide transcriptomic and physiological evidence that S may be critical for plant Hg stress resistance and will help to develop strategies for reduction or phytoremediation of Hg contamination.

关键词： Sulfur Mercury Transcriptomics Detoxification

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