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Journal of Materials Science & Technology 2023年第17期148卷 10-18页

作者： Zhao Song Lingyu Li Yidi Chen Xiaoguang Duan nanqi ren State Key Laboratory of Urban Water Resource and Environment Shenzhen Key Laboratory of Organic Pollution Prevention and ControlSchool of Civil and Environmental EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia

Biochars are low-cost and sustainable materials for environmental technologies.In this work,we pre-pared three biochars using pomelo peel(P-BC),algae(A-BC),and corncob(C-BC)to recover Cd^(2+)from wastewater via capacitive deionisation(CDI).A-BC possesses the highest amount of mesopores and nitro-gen functionality and attains the highest removal of Cd^(2+)via physical adsorption.For the electro-sorption capacity,C-BC and A-BC perform better capacitive removal of Cd^(2+)than P-BC due to the smaller charge-transfer and mass-transfer resistances.Also,this work investigated the impacts of surface morphology,cell voltage,NaCl,initial pH,and Cd^(2+)concentrations on Cd^(2+)capacitive removal and electrode regen-eration performances.The results indicated that A-BC and C-BC may be prospective materials for Cd^(2+)removal from wastewater by CDI.However,the presence of competing cations at high concentrations may influence the removal of Cd^(2+)at a low level,requiring the modification of A-BC and C-BC in future work.

关键词： Biochar Cd removal Capacitive deionisation Heavy metals Selectivity

Selective activation of peroxymonosulfate to singlet oxygen by engineering oxygen vacancy defects in Ti_(3)CNT_(x) MXene for effective removal of micropollutants in water

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Fundamental Research 2023年第5期3卷 770-776页

作者： Limin Jin Shijie You nanqi ren Yanbiao Liu College of Environmental Science and Engineering Textile Pollution Controlling Engineering Center of the Ministry of Ecology and EnvironmentDonghua University2999 North Renmin RoadShanghai 201620China State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China

Defect engineering is an effective strategy to boost the catalytic activity of MXene towards heterogeneous peroxymonosulfate(PMS)activation for water decontamination.Herein,we developed a facile approach to fine-tune the generation of oxygen vacancies(OVs)on Ti_(3)CNT_(x)crystals by Ce-doping(Ce-Ti_(3)CNT_(x))with the aim of mediating PMS activation for the degradation of micropollutants in water.By varying the dopant content,the OV concentrations of Ti_(3)CNT_(x)could be varied to enable the activation of PMS to almost 100%singlet oxygen(1O2),and hence the effective degradation of sulfamethoxazole(SMX,a model micropollutant).Various advanced characterization techniques were employed to obtain detailed information on the microstructure,morphology,and defect states of the catalysts.The experimental results showed that SMX removal was proportional to the OVs level.Density functional theory(DFT)models demonstrated that,in contrast to pristine Ti_(3)CNT_(x),the OVs on 10%CeTi_(3)CNT_(x)could adsorb the terminal O of PMS,which facilitated the formation of SO_(5)•−as well as the generation of 1O2.We further loaded the optimized catalysts onto a polytetrafluoroethylene microfiltration membrane and also demonstrated the efficient removal of SMX from water using a convection-enhanced mass transport flowthrough configuration.This study provides new insights into the effective removal of micropollutants from water by integrating state-of-the-art defect engineering,advanced oxidation,and microfiltration techniques.

关键词： Oxygen vacancy Ce-doped MXene Peroxymonosulfate activation Singlet oxygen Water decontamination

One-pot hydrothermal fabrication of BiVO_(4)/Fe_(3)O_(4)/rGO composite photocatalyst for the simulated solar light-driven degradation of Rhodamine B

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Frontiers of Environmental Science & Engineering 2022年第3期16卷 105-120页

作者： Shuangyang Zhao Chengxin Chen Jie Ding Shanshan Yang Yani Zang nanqi ren State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China

Fabrication of easily recyclable photocatalyst with excellent photocatalytic activity for degradation of organic pollutants in wastewater is highly desirable for practical application.In this study,a novel ternary magnetic photocatalyst BiVO_(4)/Fe_(3)O_(4)/reduced graphene oxide(BiVO_(4)/Fe_(3)O_(4)/rGO)was synthesized via a facile hydrothermal strategy.The BiVO_(4)/Fe_(3)O_(4) with 0.5 wt%of rGO(BiVO_(4)/Fe_(3)O_(4)/0.5%rGO)exhibited superior activity,degrading greater than 99%Rhodamine B(RhB)after 120 min solar light radiation.The surface morphology and chemical composition of BiVO_(4)/Fe_(3)O_(4)/rGO were studied by scanning electron microscopy,X-ray diffraction,X-ray photoelectron spectroscopy,UV–visible diffuse reflectance spectroscopy,Fourier transform infrared spectroscopy,and Raman spectroscopy.The free radicals scavenging experiments demonstrated that hole(h^(+))and superoxide radical(O_(2)•^(−))were the dominant species for RhB degradation over BiVO_(4)/Fe_(3)O_(4)/rGO under solar light.The reusability of this composite catalyst was also investigated after five successive runs under an external magnetic field.The BiVO_(4)/Fe_(3)O_(4)/rGO composite was easily separated,and the recycled catalyst retained high photocatalytic activity.This study demonstrates that catalyst BiVO_(4)/Fe_(3)O_(4)/rGO possessed high dye removal efficiency in water treatment with excellent recyclability from water after use.The current study provides a possibility for more practical and sustainable photocatalytic process.

关键词： Photocatalysis Ternary magnetic photocatalyst Visible-light-driven Free radicals trapping Reusability Recycling

Electrochemical Removal of Chlorophenol Pollutants by Reactive Electrode Membranes: Scale-Up Strategy for Engineered Applications

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Engineering 2022年第2期8卷 77-84页

作者： Shuzhao Pei Yi Wang Shijie You Zhanguo Li nanqi ren State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China State Key Laboratory of NBC Protection for Civilian Beijing 102205China

Chlorophenols(CPs)are significant refractory pollutants that are highly toxic to humans and other organ-isms.Reactive electrode membranes(REMs)show considerable potential in the electrochemical removal of refractory pollutants by allowing flow-through operations with convection-enhanced mass transfer.However,relevant studies are commonly performed on the laboratory scale,and there is no straightfor-ward method that guarantees success in scaling up engineered REM reactors.In this study,we demon-strated that a tubular concentric electrode(TCE)configuration with a titanium suboxide ceramic anode and a stainless-steel cathode is suitable for large-scale CPs removal.Both theoretical and experi-mental results showed that the TCE configuration not only allows the electrode surface to be orthogonal to electric field lines everywhere,but also has an ohmic resistance that is inversely proportional to the length of the electrode.In addition,the TCE configuration can be operated in either the anode-to-cathode(AC)or the cathode-to-anode(CA)mode based on the flow direction,creating adjustable condi-tions for selective degradation of CPs.This was confirmed by 98%removal of 2,4-dichlorophenol(2,4-DCP)and 72.5%removal of chemical oxygen demand(COD)in the CA mode,in which the kinetic constant was one order of magnitude higher than that for the AC mode under flow-through single-pass operations.This can be explained by the lower activation energy and free energy in the CA mode,as revealed by the-oretical calculations and experimental measurements.The TCE configuration is also suitable for a numbering-up strategy to scale up the electrochemical reactor without increasing the ohmic resistance or decreasing the specific electrode area,achieving 99.4%removal of 2,4-DCP with an energy consump-tion of 1.5 kW·h·m^(-3) when three TCE modules were employed.This study presents a suitable electrode design configuration for the REM reactor,offering effective strategies to bridge the“Valley of Death”encountered when scaling up the electrochemica

关键词： Chlorophenols Reactive electrode membrane Tubular concentric electrode Scale-up

Carbon neutrality of wastewater treatment-A systematic concept beyond the plant boundary

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Environmental Science and Ecotechnology 2022年第3期11卷 57-63页

作者： Lanqing Li Xiuheng Wang Jingyu Miao Aliya Abulimiti Xinsheng Jing nanqi ren State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin150090PR China School of Civil and Environmental Engineering Harbin Institute of Technology(Shenzhen)Shenzhen518055China

Recently,every industry has been working to achieve carbon neutrality,and the wastewater sector is no exception.However,little research focuses on the carbon accounting of wastewater treatment and the roadmap to carbon neutrality.Here,to systematically perform accounting,we provide a sketch that describes three boundaries of the wastewater system and propose that the carbon neutrality of the wastewater system is far beyond the plant boundary.Moreover,we identify the direct and indirect carbon emissions of wastewater treatment.In addition to direct emissions of CH_(4) and N_(2)O,direct fossil CO_(2) emissions from wastewater treatment should be included in accounting to set accurate guidelines.Next,the technologies that assist in achieving carbon-neutral wastewater treatment both within-thefence of wastewater treatment plants and beyond the plant boundary are summarized.All measurements of energy recovery,resource recovery,and water reuse contribute to reaching this goal.The concepts of energy neutrality and carbon neutrality are identified.Successful wastewater treatment cases in energy self-sufficiency may not achieve carbon neutrality.Meanwhile,resource recovery methods are encouraged,especially to produce carbon-based materials.Ultimately,the trend of preference for the decentralized sewage treatment system is pinpointed,and systematic thinking to set the urban infrastructure layout as a whole is advocated.

关键词： Carbon neutrality Wastewater treatment Fossil CO_(2)emissions System boundaries Systematic thinking

Sustainable Generation of Sulfate Radicals and Decontamination of Micropollutants via Sequential Electrochemistry

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Engineering 2023年第11期30卷 144-152页

作者： Wentian Zheng Shijie You Yuan Yao nanqi ren Bin Ding Fang Li Yanbiao Liu College of Environmental Science and Engineering Donghua UniversityShanghai 201620China State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150080China Innovation Center for Textile Science and Technology College of TextilesDonghua UniversityShanghai 200051China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

The removal of emerging micropollutants in the aquatic environment remains a global challenge.Conventional routes are often chemically,energetically,and operationally intensive,which decreases their sustainability during applications.Herein,we develop an advanced chemical-free strategy for micropollutants decontamination that is solely based on sequential electrochemistry involving ubiquitous sulfate anions in natural and engineered waters.This can be achieved via a chain reaction initiated by electrocatalytic anodic sulfate(SO_(4)^(2-))oxidation to produce persulfate(S_(2)O_(8)^(2-))and followed by a cathodic persulfate reduction to produce sulfate radicals(SO_(4)^(·-)).These SO_(4)^(·-)are powerful reactive species that enable the unselective degradation of micropollutants and yield SO_(4)^(2-)again in the treated water.The proposed flow-through electrochemical system achieves the efficient degradation(100.0%)and total organic carbon removal(65.0%)of aniline under optimized conditions with a single-pass mode.We also reveal the effectiveness of the proposed system for the degradation of a wide array of emerging micropollutants over a broad pH range and in complex matrices.This work provides the first proof-ofconcept demonstration using ubiquitous sulfate for micropollutants decontamination,making water purification more sustainable and more economical.

关键词： Advanced oxidation Chain reaction Sulfate radical Micropollutants Sequential electrochemistry

Preparation and characterization of a lipoid adsorption material and its atrazine removal performance

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Journal of Environmental Sciences 2011年第8期23卷 1293-1298页

作者： Zhiqiang Chen Qinxue Wen Jiaxiang Lian nanqi ren State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology Harbin 150090 China. National Engineering Research Center of Urban Water Resources Harbin Institute of Technology Harbin 150090 China

A novel adsorbent named lipold adsorption material （LAM）, with a hydrophoblc nucleolus （trlolem） and a hydrophlllc membrane structure （polyamide）, was synthesized to remove hydrophobic organic chemicals （HOCs） from solution. Triolein, a type of lipoid, was entrapped by the polyamide membrane through an interfacial polymerization reaction. The method of preparation and the structure of the LAM were investigated and subsequent experiments were conducted to determine the characteristics of atrazine （a type of HOC） removal from wastewater using LAM as the adsorbent. The results showed that LAM had a regular structure compared with the prepolymer, where compact particles were linked with each other and openings were present in the structure of the LAM in which the fat drops formed from triolein were entrapped. In contrast to the atrazine adsorption behavior of powdered activated carbon （PAC）, LAM showed a persistent adsorption capacity for atrazine when initial concentrations of 0.57, 1.12, 8.31 and 19.01 mg/L were present, and the equilibrium time was 12 hr. Using an 8 mg/L initial concentration of atrazine as an indicator of HOCs in aqueous solution, experiments on the adsorption capacity of the LAM showed 69.3% removal within 6-12 hr contact time, which was close to the 75.5% removal of atrazine by PAC. Results indicated that LAM has two atrazine removal mechanisms, namely the bioaccumulation of atrazine by the nucleous material and physical adsorption to the LAM membrane. Bioaccumulation was the main removal mechanism.

关键词： lipoid adsorption material atrazine powdered activated carbon

Bulking sludge for PHA production:Energy saving and comparative storage capacity with well-settled sludge

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Journal of Environmental Sciences 2012年第10期24卷 1744-1752页

作者： Qinxue Wen Zhiqiang Chen Changyong Wang nanqi ren State Key Laboratory of Urban Water Resource and Environment Harbin Institute of TechnologyHarbin 150090China

Two acetate-fed sequencing batch reactors （SBR） were operated under an aerobic dynamic feeding （ADF） model （SBR#2） and with anaerobic phase before aerobic phase （SBR#1） to select mixed cultures with a high polyhydroxyalkanoates （PHA） storage response. Although kinetic selection based on storage response should bring about a predominance of floc-formers, a bulking sludge with storage response comparable to well-settled sludge was steadily established. An anaerobic phase was introduced before the aerobic phase in the ADF model to improve the sludge settleability （SBR #1）, however, due to the consequent increased feast/famine ratio, the performance of SBR #1, in terms of both the maximum PHB （polyhydroxybutyrate） cell content and APHB, was lower than that of SBR #2. SBR #2 gradually reached a steady state while SBR #1 failed suddenly after 50 days of operation. The maximum specific substrate uptake rate and storage rate for the selected bulking sludge were 0.4 Cmol Ae/（Cmol X.hr） and 0.18 Cmol Ac/（Cmol PHB.hr）, respectively, resulting a yield of 0.45 Cmol PHB/（Cmol Ae） in SBR #2 in the culture enrichment phase. A maximum PHB content of 53% of total suspended solids and PHB storage rate of 1.36 Cmol Ac/（Cmol PHB.hr） was achieved at 10.2 hr in batch accumulation tests under nitrogen starvation. The results indicated that it was feasible to utilize filamentous bacteria to accumulate PHA with a rate comparable to well-settled sludge, Furthermore, the lower dissolved oxygen demand of filamentous bacteria would save energy required for aeration in the culture enrichment stage.

关键词： polyhydroxyalkanoates mixed cultures aerobic dynamic feeding bulking sludge feast/famine ratio

Biodegradation of phenol and m-cresol by mutated Candida tropicalis

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Journal of Environmental Sciences 2010年第4期22卷 621-626页

作者： Yan Jiang Xun Cai Di Wu nanqi ren State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology Harbin 150090 China. Department of Chemical Engineering Daqing Oilfield Engineering Limited Company Daqing 163712 China School of Life Sciences and Chemistry Harbin University Harbin 150016 China

The phenol and m-cresol biodegradations were studied using the mutant strain CTM 2 obtained by the He-Ne laser irradiation on wild-type Candida tropicalis. The results showed that C. tropicalis exhibited the increased capacity of phenolic compounds degradation after laser irradiation. It could degrade 2600 mg/L phenol and 300 mg/L m-cresol by 5% inoculum concentration, respectively. In the dual-substrate biodegradation system, 0-500 mg/L phenol could accelerate m-cresol biodegradation, and 300 mg/L m-cresol could be completely utilized within 46 hr at the presence of 350 mg/L phenol. Besides, the maximum biodegradation of m-cresol could reach 350 mg/L with 80 mg/L phenol within 61 hr. Obviously, phenol, as a growth substrate, could promote CTM 2 to degrade m-cresol, and was always preferentially utilized as carbon source. Comparatively, low-concentration m-cresol could result in a great inhibition on phenol degradation. In addition, the kinetic behaviors of cell growth and substrate biodegradation were described by kinetic model proposed in our laboratory.

关键词： biodegradation the mutant strain CTM 2 phenol m-cresol kinetic

Effect of temperature switchover on the degradation of antibiotic chloramphenicol by biocathode bioelectrochemical system

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Journal of Environmental Sciences 2014年第8期26卷 1689-1697页

作者： Deyong Kong Bin Liang Duu-Jong Lee Aijie Wang nanqi ren State Key Laboratory of Urban Water Resource and Environment School of Municipal and Environmental EngineeringHarbin Institute of Technology Key laboratory of Environmental Biotechnology Research Center for Eco-Environmental SciencesChinese Academy of Sciences

Exposure to chloramphenicol（CAP）,a chlorinated nitroaromatic antibiotic,can induce CAP-resistant bacteria/genes in diverse environments. A biocathode bioelectrochemical system（BES） was applied to reduce CAP under switched operational temperatures.When switching from 25 to 10°C,the CAP reduction rate（kCAP） and the maximum amount of the dechlorinated reduced amine product（AMCl,with no antibacterial activity） by the biocathode communities were both markedly decreased. The acetate and ethanol yield from cathodophilic microbial glucose fermentation（with release of electrons） was also reduced. Formation of the product AMCl was enhanced by the biocathode dechloridation reaction compared with that produced from pure electrochemical or microbial dechloridation processes. The electrochemical and morphological analyses of cathode biofilms demonstrated that some cathodophilic microbes could adapt to low temperature and play a key role in CAP degradation. The resilient biocathode BES has a potential for the treatment of CAP-containing wastewater in temperature fluctuating environments.

关键词： Chloramphenicol degradation,Biocathode,Dechloridation,Temperature switchover