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In-situ construction of abundant active centers on hierarchically porous carbon electrode toward high-performance phosphate electrosorption: Synergistic effect of electric field and capture sites

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Green Energy & Environment 2024年第1期9卷 126-137页

作者： Peng Zhang Fukuan Li Mingming He Silu Huo Xueli Zhang Benqiang Cen Dezhi Fang Kexun Li Hao Wang College of Environmental Science and Engineering Nankai UniversityTianjin300350China MOE Key laboratory of pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlTianjin Key Laboratory of Environmental Technology for Complex Trans-Media PollutionNankai UniversityTianjin300350China State Key laboratory of Simulation and Regulation of water Cycles in River Basins China Institute of Water Resources and Hydropower ResearchBeijing100038China

Phosphate removal is crucial for eutrophication control and water quality improvement.Electro-assisted adsorption,an eco-friendly elec-trosorption process,exhibited a promising potential for wastewater treatment.However,there are few works focused on phosphate electro-sorption,and reported electrodes cannot attach satisfactory removal capacities and rates.Herein,electro-assisted adsorption of phosphate via in-situ construction of La active centers on hierarchically porous carbon(LaPC)has been originally demonstrated.The resulted LaPC composite not only possessed a hierarchically porous structure with uniformly dispersed La active sites,but also provided good conductivity for interfacial electron transfer.The LaPC electrode achieved an ultrahigh phosphate electrosorption capability of 462.01 mg g^(-1) at 1 V,outperforming most existing electrodes.The superior phosphate removal performance originates from abundant active centers formed by the coupling of electricﬁeld and capture sites.Besides,the stability and selectivity toward phosphate capture were maintained well even under comprehensive conditions.Moreover,a series of kinetics and isotherms models were employed to validate the electrosorption process.This work demonstrates a deep understanding and promotes a new level of phosphate electrosorption.

关键词： Electro-assisted adsorption Electrosorption Phosphate removal Active centers MOF-derived carbon

Colloid-facilitated release of polybrominated diphenyl ethers at an e-waste recycling site: evidence from undisturbed soil core leaching experiments

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Frontiers of Environmental Science & Engineering 2024年第2期18卷 91-101页

作者： Zebin Huo Mengjun Xi Lianrui Xu Chuanjia Jiang Wei Chen College of Environmental Science and Engineering Ministry of Education Key Laboratory of Pollution Processes and Environmental CriteriaTianjin Key Laboratory of Environmental Remediation and Pollution ControlNankai UniversityTianjin 300350China

Polybrominated diphenyl ethers (PBDEs), a class of persistent organic pollutants, have been frequently detected in soil at e-waste recycling sites. However, the key factors controlling the transport of PBDEs from surface soil to the vadose zone and groundwater are unclear. Here, colloid-enhanced leaching of PBDEs from undisturbed soil cores collected at an e-waste recycling site in Tianjin, China, is reported. Spatially heterogeneous release of colloids and PBDEs was observed in all the tested soil cores under chemical and hydrodynamic perturbations, indicating the presence of preferential flow paths. Colloid concentration in the effluent significantly increased as ionic strength decreased (from 10 to 0.01 mmol/L), probably due to the stronger electrostatic repulsion between colloidal particles and the soil matrix at lower ionic strength. In contrast, colloid mobilization was not significantly affected by the changes in pH of the influent (from 4.0 to 10.0) and flow rate (from a Darcy velocity of 1.5 to 6.0 cm/h). The concentrations of 2,2′,3,3′,4,4′,5,5′,6,6′-decabromodiphenyl ether (BDE-209), the predominant PBDE congener at the site, detected in the leachate (ranging from 1.09 to 3.43 ng/L) were much lower than previously reported results from packed column leaching tests, and were positively correlated with colloid concentrations. This indicates that remobilization of colloids at e-waste recycling sites can promote the leaching and downward migration of PBDEs from surface soil. The findings highlight the potential risk of surface soil PBDE contamination to groundwater quality and call for further understanding of colloid-facilitated transport for predicting the fate of PBDEs at e-waste recycling sites.

关键词： Polybrominated diphenyl ether Colloid-facilitated transport E-waste recycling site Undisturbed soil core Groundwater quality

A Unifi ed View of Carbon Neutrality:Solar-Driven Selective Upcycling of Waste Plastics

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Transactions of Tianjin University 2024年第1期30卷 1-26页

作者： Zhiyong Zhao Shuai Yue Gaohua Yang Pengfei Wang Sihui Zhan MOE Key laboratory of pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlCollege of Environmental Science and EngineeringTianjin 300350China

With the rapid development of plastic production and consumption globally,the amount of post-consumer plastic waste has reached levels that have posed environmental threats.Considering the substantial CO_(2)emissions throughout the plastic lifecycle from material production to its disposal,photocatalysis is considered a promising strategy for eff ective plastic recycling and upcycling.It can upgrade plastics into value-added products under mild conditions using solar energy,realizing zero carbon emissions.In this paper,we explain the basics of photocatalytic plastic reformation and underscores plastic feedstock reformation pathways into high-value-added products,including both degradation into CO_(2)followed by reformation and direct reformation into high-value-added products.Finally,the current applications of transforming plastic waste into fuels,chemicals,and carbon materials and the outlook on upcycling plastic waste by photocatalysis are presented,facilitating the realization of carbon neutrality and zero plastic waste.

关键词： Photocatalysis Photoreforming Plastics upcycling Carbon neutrality Energy storage and conversion

Tailoring the surface and interface structures of photocatalysts to enhance hydrogen production

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Science China Chemistry 2024年第4期67卷 1161-1174页

作者： Tao Zhang Pengfei Wang Shuai Yue Fei Li Zhiyong Zhao Sihui Zhan MOE Key laboratory of pollution Processes and Environmental Criteria/Tianjin Key laboratory of Environmental remediation and pollution Control College of Environmental Science and EngineeringNankai UniversityTianjin 300350China

Photocatalytic water splitting using semiconductor photocatalysts is a promising approach for the production of carbon-neutral,sustainable and clean hydrogen fuel.However,the separation and transport of photoinduced carriers are generally considered to be rate-limiting steps,and their low efficiency remains a major challenge.Therefore,much effort has been devoted to developing new strategies in surface/interface engineering of photocatalysts to improve the dynamics of charge separation/transport.This feature article briefly summarizes recent advances in photocatalyst surface/interface engineering by our research group,which have been achieved through the design of various novel photocatalysts,including interfacial modulation,heterostructure construction,heteroatom doping,single atom and diatom sites.The article is divided into three parts:first,we briefly introduce the three key processes involved in solar water splitting and reveal relationships between the properties of nanostructural photocatalysts and the fundamentals of water splitting;second,we detail methods and strategies for surface and interfacial structures to improve the efficiency of the fundamental processes,especially charge separation;finally,we explore prospects for photocatalytic water splitting applications.This article provides a valuable resource and strategies for researchers currently working in the field of photocatalytic water splitting.

关键词： photocatalytic water splitting surface/interface structures dual-functional photocatalysis

Strategies of selective electroreduction of aqueous nitrate to N_(2) in chloride-free system:A critical review

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Green Energy & Environment 2024年第2期9卷 198-216页

作者： Fukuan Li Weizhe Zhang Peng Zhang Ao Gong Kexun Li College of Environmental Science and Engineering Nankai UniversityTianjin300350China MOE Key laboratory of pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlTianjin Key Laboratory of Environmental Technology for Complex Trans-Media PollutionNankai UniversityTianjin300350China

Electroreduction of nitrate has been gaining wide attention in recent years owing to it's beneficial for converting nitrate into benign N_(2) from the perspective of electrocatalytic denitrification or into value-added ammonia from the perspective of electrocatalytic NH_(3) synthesis.By reason of the undesired formation of ammonia is dominant during electroreduction of nitrate-containing wastewater,chloride has been widely used to improve N_(2) selectivity.Nevertheless,selective electroreduction of nitrate to N2 gas in chloride-containing system poses several drawbacks.In this review,we focus on the key strategies for efficiently enhancing N_(2) selectivity of electroreduction of nitrate in chloride-free system,including optimal selection of elements,combining an active metal catalyst with another metal,manipulating the crystalline morphology and facet orientation,constructing core–shell structure catalysts,etc.Before summarizing the strategies,four possible reaction pathways of electro-reduction of nitrate to N_(2) are discussed.Overall,this review attempts to provide practical strategies for enhancing N2 selectivity without the aid of electrochlorination and highlight directions for future research for designing appropriate electrocatalyst for final electrocatalytic denitrifi-cation.

关键词： Nitrate Chloride Electroreduction Selectivity Nitrogen

Challenges and perspectives of air pollution control in China

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Frontiers of Environmental Science & Engineering 2024年第6期18卷 9-16页

作者： Bin Zhao Shuxiao Wang Jiming Hao State Key Joint laboratory of Environmental Simulation and pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China State Environmental Protection Key laboratory of Sources and Control of Air pollution Complex Beijing 100084China

Air pollution is one of the most challenging environmental issues in the world.China has achieved remarkable success in improving air quality in last decade as a result of aggressive air pollution control policies.However,the average fine particulate matter(PM2.5)concentration in China is still about six times of the World Health Organization(WHO)Global Air Quality Guidelines(AQG)and causing significant human health risks.Extreme emission reductions of multiple air pollutants are required for China to achieve the AQG.Here we identify the major challenges in future air quality improvement and propose corresponding control strategies.The main challenges include the persistently high health risk attributed to PM2.5 pollution,the excessively loose air quality standards,and coordinated control of air pollution,greenhouse gases(GHGs)emissions and emerging pollutants.To further improve air quality and protect human health,a health-oriented air pollution control strategy shall be implemented by tightening the air quality standards as well as optimizing emission reduction pathways based on the health risks of various sources.In the meantime,an“oneatmosphere”concept shall be adopted to strengthen the synergistic control of air pollutants and GHGs and the control of non-combustion sources and emerging pollutants shall be enhanced.

关键词： Air pollution China Health impact Air quality standards GHGs Emerging pollutants

Boosting oxygen vacancies by modulating the morphology of Au decorated In_(2)O_(3)with enhanced CO_(2)hydrogenation activity to CH_(3)OH

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Journal of Environmental Sciences 2024年第6期140卷 91-102页

作者： Ruxian Hou Jiewen Xiao Qian Wu Tianyu Zhang Qiang Wang Beijing Key Lab for Source Control Technology of water pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China Engineering Research Center for water pollution Source Control&Eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China

CO_(2)hydrogenation to methanol has become one of the most promising ways for CO_(2)utilization,however,the CO_(2)conversion rate and methanol selectivity of this reaction still need to be improved for industrial application.Here we investigated the structure-activity relationship for CO_(2)conversion to methanol of In_(2)O_(3)-based catalysts by modulating morphology and decorating Au.Three different Au/In_(2)O_(3)catalysts were prepared,their activity follow the sequence of Au/In_(2)O_(3)-nanosphere(Au/In_(2)O_(3)-NS)>Au/In_(2)O_(3)-nanoplate(Au/In_(2)O_(3)-NP)>Au/In_(2)O_(3)-hollow microsphere(Au/In_(2)O_(3)-HM).Au/In_(2)O_(3)-NS exhibited the best performance with good CO_(2)conversion of 12.7%,high methanol selectivity of 59.8%,and large space time yield of 0.32 g CH_(3)OH/(hr·gcat)at 300℃.The high performance of Au/In_(2)O_(3)-NS was considered as the presence of Au.It contributes to the creation of more surface oxygen vacancies,which further promoted the CO_(2)adsorption and facilitated CO_(2)activation to form the formate intermediates towards methanol.This work clearly suggests that the activity of In_(2)O_(3)catalyst can be effective enhanced by structure engineering and Au decorating.

关键词： CO_(2)hydrogenation Methanol Au/In_(2)O_(3) Morphology Oxygen vacancies

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 wastewater.This 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)shell.The 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),respectively.The 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 observed.The 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 efficiency.Therefore,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

Calcium-based polymers for suppression of soil acidification by improving acid-buffering capacity and inhibiting nitrification

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Journal of Environmental Sciences 2024年第5期139卷 138-149页

作者： Fei Kang Yunshan Meng Yanning Ge Yun Zhang Haixiang Gao Xueqin Ren Jie Wang Shuwen Hu Beijing Key laboratory of Farmland Soil pollution Prevention-control and remediation College of Resources and Environmental SciencesChina Agricultural UniversityBeijing 100193China Department of Applied Chemistry China Agricultural UniversityBeijing 100193China

Soil acidification is a major threat to agricultural sustainability in tropical and subtropical regions.Biodegradable and environmentally friendly materials,such as calcium lignosulfonate(CaLS),calcium poly(aspartic acid)(PASP-Ca),and calcium polyγ-glutamic acid(γ-PGA-Ca),are known to effectively ameliorate soil acidity.However,their effectiveness in inhibiting soil acidification has not been studied.This study aimed to evaluate the effect of CaLS,PASP-Ca,andγ-PGA-Ca on the resistance of soil toward acidification as directly and indirectly(i.e.,via nitrification)caused by the application of HNO_(3)and urea,respectively.For comparison,Ca(OH)_(2)and lignin were used as the inorganic and organic controls,respectively.Among the materials,γ-PGA-Ca drove the substantial improvements in the pH buffering capacity(pHBC)of the soil and exhibited the greatest potential in inhibiting HNO_(3)-induced soil acidification via protonation of carboxyl,complexing with Al~(3+),and cation exchange processes.Under acidification induced by urea,CaLS was the optimal one in inhibiting acidification and increasing exchangeable acidity during incubation.Furthermore,the sharp reduction in the population sizes of ammonia-oxidizing bacteria(AOB)and ammonia-oxidizing archaea(AOA)confirmed the inhibition of nitrification via CaLS application.Therefore,compared to improving soil pHBC,CaLS may play a more important role in suppressing indirect acidification.Overall,γ-PGA-Ca was superior to PASP-Ca and CaLS in enhancing the soil pHBC and the its resistance to acidification induced by HNO_(3) addition,whereas CaLS was the best at suppressing urea-driven soil acidification by inhibiting nitrification.In conclusion,these results provide a reference for inhibiting soil re-acidification in intensive agricultural systems.

关键词： Calcium-based polymer Soil acidification pH buffering capacity Nitrification inhibition