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Simple preparation of C(CS)/g-C_(3)N_(4)/Co carbon aerogel and its catalytic performance for ammonium perchlorate

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Defence Technology（防务技术） 2024年第3期33卷 186-196页

作者： Yujie Yan Bo Jin Rufang Peng State Key Laboratory of environment-friendly energy Materials School of Materials Science and EngineeringSouthwest University of Science and TechnologyMianyang621010China

Biomass chitosan(CS)was used as a template,graphitic phase carbon nitride(g-C_(3)N_(4))with high nitrogen content and certain catalytic activity was used as a dopant,and nano-transition metal cobalt(Co)was used as a catalytic center point.The carbon aerogel(C(CS)/g-C_(3)N_(4)/Co)with a three-dimensional network-like structure was prepared by assembling the three materials through experimental operations such as freeze-drying and high-temperature carbonization.It was demonstrated by scanning and transmission characterization that the CS in the carbon aerogel could provide more active sites for the cobalt nanoparticles,and the doping of graphite-phase carbon nitride as a template dispersed the cobalt nanoparticles and changed the conductivity of the CS.To investigate the catalytic effect of carbon aerogel on ammonium perchlorate(AP),it was investigated by differential thermal analyzer and TG thermal analysis.This carbon aerogel was very effective in catalyzing AP,and the 10 wt% content of the catalyst reduced the AP pyrolysis peak from 703.9 to 595.5 K.And to further investigate the synergistic effect of the three materials,further carbon aerogels such as C(CS)/Co,g-C_(3)N_(4)/Co were prepared and applied to catalyze AP,and the same ratio reduced the AP pyrolysis peak by 98.1℃ and 97.7℃.This result indicates a synergistic effect of the assembly of the three materials.

关键词： g-C_(3)N_(4) Chitosan Co Ammonium perchlorate Pyrolysis kinetics

Remediation of di(2-ethylhexyl)phthalate(DEHP)contaminated black soil by freeze-thaw aging biochar

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Journal of environmental Sciences 2024年第1期135卷 681-692页

作者： Lei Wang Zeyu Dou Chaoran Ma Xiaochen Jia Hongye Wang Wenjing Bao Lei Wang Jianhua Qu Ying Zhang school of Resources and environment Northeast Agricultural UniversityHarbin 150030China

Di(2-ethylhexyl)phthalate(DEHP),a complex structure with high toxicity,is a common organic pollutant.This study investigated the effects of fresh biochar(FBC),and freeze-thaw cycled aged biochar(FTC-BC)on DEHP-contaminated soils using a pot experiment.The specific surface area of FBC increased from 145.20 to 303.50 m~2/g,and oxygen-containing functional groups increased from 1.26 to 1.48 mol/g after freeze-thaw cycles,greatly enhancing the adsorption of DEHP by biochar in the soil.The comprehensive radar chart evaluation showed that FBC and FTC-BC reduced DEHP growth stress and improved the soil properties.Compared with FBC,FTC-BC performed better in protecting the normal growth of pakchoi and improving soil properties.In addition,the application of biochar increased the diversity and abundance of bacteria in the DEHP-contaminated soil and changed the composition of the soil bacterial community.The partial least squares path model(PLS-PM)showed that adding biochar as a soil remediation agent significantly positively impacted soil nutrients and indirectly reduced the DEHP levels in soil and plants by increasing soil microbial diversity.Compared with FBC,FTC-BC creates a more satisfactory living environment for microorganisms and has a better effect on the degradation of DEHP in the soil.This study provides a theoretical basis for future biochar remediation of DEHP-contaminated soils in cold high-latitude regions.

关键词： DEHP Freeze-thaw cycles Biochar Soil restoration

A combined evaluation of the characteristics and antibiotic resistance induction potential of antibiotic wastewater during the treatment process

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Journal of environmental Sciences 2024年第4期138卷 626-636页

作者： Sun Miao Yanyan Zhang Cong Men Yiou Mao Jiane Zuo State Key Joint Laboratory of environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China school of energy and environmental Engineering Beijing Key Laboratory of Resource-Oriented Treatment of Industrial PollutantsUniversity of Science and Technology BeijingBeijing 100083China High school Affiliated to Renmin University of China Beijing 100080China Tsinghua Shenzhen International Graduate school Shenzhen 518055China

Antibiotic wastewater contains a variety of pollutant stressors that can induce and promote antibiotic resistance(AR)when released into the environment.Although these substances are mostly in concentrations lower than those known to induce AR individually,it is possible that antibiotic wastewater discharge might still promote the AR transmission risk via additive or synergistic effects.However,the comprehensive effect of antibiotic wastewater on AR development has rarely been evaluated,and its treatment efficiency remains unknown.Here,samples were collected from different stages of a cephalosporin production wastewater treatment plant,and the potential AR induction effect of their chemical mixtures was explored through the exposure of the antibiotic-sensitive Escherichia coli K12 strain.Incubation with raw cephalosporin production wastewater significantly promoted mutation rates(3.6×10^(3)-9.3×10^(3)-fold)and minimum inhibition concentrations(6.0-6.7-fold)of E.coli against ampicillin and chloramphenicol.This may be attributed to the inhibition effect and oxidative stress of cephalosporin wastewater on E.coli.The AR induction effect of cephalosporin wastewater decreased after the coagulation sedimentation treatment and was completely removed after the full treatment process.A Pearson correlation analysis revealed that the reduction in the AR induction effect had a strong positive correlation with the removal of organics and biological toxicity.This indicates that the antibiotic wastewater treatment had a collaborative processing effect of conventional pollutants,toxicity,and the AR induction effect.This study illustrates the potential AR transmission risk of antibiotic wastewater and highlights the need for its adequate treatment.

关键词： Antibiotic wastewater treatment plant Antibiotic resistance Antibiotic resistance induction effect Correlation analysis Biological toxicity

Three-dimensionally ordered macroporous(3DOM) structure promoted the activity and H_(2)O poisoning resistance of Ce Mn/3DOM-TiO_(2) catalyst in NH_(3)-SCR

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Journal of Rare Earths 2024年第3期42卷 523-533,I0004页

作者： Yaqin Hu Shipeng Ding Chenchen Tan Peng Wu Guobo Li Sheng Wang Hongqiang Yang Yaping Zhang Key Laboratory of energy Thermal Conversion and Control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing210096China State Power environmental Protection Research Institute Nanjing210031China

NH_(3)-SCR is an effective mean of NOxremoval in the non-electric industry, however, the high activation temperature and poor H_(2)O resistance of SCR catalysts posed a barrier to its application. In this work, a series of three-dimensionally ordered macroporous(3DOM) catalysts were synthesized via a colloidal crystal template(CCT) method, and various characterizations were carried out to explore the physicochemical property of catalysts. The experiment results reveal that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst presents the excellent low-temperature catalytic activity of nearly 100% at 100℃. Furthermore, the enhanced H_(2)O resistance is achieved, certified by the unaffected NO remove at 150℃ in the participation of 15 vol% H_(2)O. The characterizations results exhibit that the improved dispersion of the active component and enhanced redox ability are conducive to the low-temperature catalytic activity. N_(2) adsorption and desorption experiments indicate that catalyst with 3DOM support possesses a larger pore diameter and specific surface area, which may weaken the condensation of H_(2)O in the microporosity of catalysts and improved the H_(2)O resistance of the catalyst. In situ DRIFTS results manifest that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst could not only absorb more NH_(3) and generate more surface-active sites, but inhibit the competitive adsorption between H_(2)O and SCR reactants.

关键词： 3DOM material NH_(3)-SCR H_(2)O resistance Low-temperature Cerium Rare earths

The response of structure and nitrogen removal function of the biofilm on submerged macrophytes to high ammonium in constructed wetlands

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Journal of environmental Sciences 2024年第8期142卷 129-141页

作者： Xue Jiang Mengmeng Wang Shunqing Yang Di He Fei Fang Liuyan Yang State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China school of Resources and environment Anqing Normal UniversityAnqing 246133China

The ammonium exceedance discharge from sewage treatment plants has a great risk to the stable operation of subsequent constructed wetlands(CWs).The effects of high ammonium shocks on submerged macrophytes and epiphytic biofilms on the leaves of submerged macrophytes in CWs were rarely mentioned in previous studies.In this paper,the 16S rRNA sequencing method was used to investigate the variation of the microbial communities in biofilms on the leaves of Vallisneria natans plants while the growth characteristics of V.natans plants were measured at different initial ammonium concentrations.The results demonstrated that the total chlorophyll and soluble sugar synthesis of V.natans plants decreased by 51.45%and 57.16%,respectively,and malondialdehyde content increased threefold after8 days if the initial NH_(4)^(+)-N concentration was more than 5 mg/L.Algal density,bacterial quantity,dissolved oxygen,and pH increased with high ammonium shocks.The average removal efficiencies of total nitrogen and NH_(4)^(+)-N reached 73.26%and 83.94%,respectively.The heat map and relative abundance analysis represented that the relative abundances of phyla Proteobacteria,Cyanobacteria,and Bacteroidetes increased.The numbers of autotrophic nitrifiers and heterotrophic nitrification aerobic denitrification(HNAD)bacteria expanded in biofilms.In particular,HNAD bacteria of Flavobacterium,Hydrogenophaga,Acidovorax,Acinetobacter,Pseudomonas,Aeromonas,and Azospira had higher abundances than autotrophic nitrifiers because there were organic matters secreted from declining leaves of V.natans plants.The analysis of the nitrogen metabolic pathway showed aerobic denitrification was the main nitrogen removal pathway.Thus,the nitrification and denitrification bacterial communities increased in epiphytic biofilms on submerged macrophytes in constructed wetlands while submerged macrophytes declined under ammonium shock loading.

关键词： Ammonium shock loading Biofilm Autotrophic nitrifiers Heterotrophic nitrification aerobic denitrification bacteria Submerged macrophyte

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

The risk factors and threshold level of subchronic inhalation exposure of reclaimed water

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Journal of environmental Sciences 2024年第3期137卷 639-650页

作者： Jiayang Kong Yun Lu Yunru Ren Menghao Chen Gang Liu Liangliang Shi State Key Joint Laboratory of environment Simulation and Pollution Control State Environment Protection Key Laboratory of Microorganism Application and Risk ControlSchool of EnvironmentTsinghua UniversityBeijing 100084China

Inhalation of reclaimed water is known to cause lung infammation,and free endotoxins have been shown to be a major risk factor for acute exposure.Subchronic exposure has also been shown to induce infammatory responses with visible tissue damage.However,subchronic risk factors have yet to be identified,and a threshold for the protection of occupational populations during urban reuse is necessary.In this study,potential risk factors in reclaimed water were examined by subchronic exposure with fractionated reclaimed water,and the health risk threshold was tested with a series of diluted reclaimed water.Accordingly,following a 12-week exposure,macromolecules and microorganisms were found to be two major risk factors in reclaimed water that could cause pulmonary infammation,including increased proportion of polymorphonuclear leukocytes in bronchoalveolar fuid,formation of inducible bronchus-associated lymphoid tissue,and elevation of Immunoglobulin A levels.Moreover,infammation persisted after a 4-week recovery period.The calculated threshold of reclaimed water exposure for mice was 31.8 Endotoxin Unit(EU)/(kg·day)under when exposed to 50%additional relative humidity from reclaimed water at 25℃ for 2 hr/day.Meanwhile,the subchronic threshold estimate for humans under the same exposure conditions was found to be 12.2 EU/(kg·day),corresponding to endotoxin levels of 61.7 EU/mL in reclaimed water.The threshold level of endotoxin was lower than that in most non-potable reclaimed water.The findings of this study suggest that occupational exposure of reclaimed water can serve as a potential risk to workers.

关键词： Reclaimed water Inhalation exposure Risk factor Threshold Infammation Endotoxin

Plastic Crystal Neopentyl Glycol/Multiwall Carbon Nanotubes Composites for Highly Efficient Barocaloric Refrigeration System

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Journal of Thermal Science 2024年第1期33卷 383-393页

作者： DAI Zhaofeng SHE Xiaohui SHAO Bohan YIN Ershuai DING Yulong LI Yongliang ZHANG Xiaosong ZHAO Dongliang school of energy&environment Southeast UniversityNanjing 210096China school of Mechanical Engineering Shijiazhuang Tiedao UniversityShijiazhuang 050043China school of energy and Power Engineering Nanjing University of Science&TechnologyNanjing 210094China Birmingham Centre for energy Storage School of Chemical EngineeringUniversity of BirminghamBirmingham B152TTUK

Plastic crystal neopentyl glycol(NPG)exhibits colossal barocaloric effect with high entropy changes.However,their application is restricted in several aspects,such as low thermal conductivity,substantial supercooling effect,and poor springback properties.In this work,multi-walled carbon nanotubes(MWCNTs)with ultra-high thermal conductivity and high mechanical strength were selected for performance enhancement of NPG.The optimal mixing ratio was determined to be NPG with 3 wt%MWCNTs composites,which showed a 6K reduction in supercooling without affecting the phase change enthalpy.Subsequently,comprehensive performance of the composites with optimal mixing ratio was compared with pure NPG At 40 MPa,390J·K^(-1)·kg^(-1)change in entropy and 9.9 K change in temperature were observed.Furthermore,the minimum driving pressure required to achieve reversible barocaloric effect was reduced by 19.2%.In addition,the thermal conductivity of the composite was increased by approximately 28%,significantly reducing the heat exchange time during a barocaloric refrigeration cycle.More importantly,ultra-high pressure release rate resulted in a73.7%reduction in the springback time of the composites,offering new opportunities for the recovery of expansion work.

关键词： barocaloric refrigeration neopentyl glycol MWCNTs performance enhancement

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 devices.Its practical application,however,is limited by the non-availability of low-cost catalysts with high activity and N_(2) selectivity.Here,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^(+))sites.The obtained Cu/NCNT-AW catalyst demonstrated outstanding activity with a T_(50)(i.***.the 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 literature.Reaction 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 intermediate.According 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 N-dopants.Specifically,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 catalyst.This 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