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Research progress of graphene-based nanomaterials for the environmental remediation

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Chinese Chemical Letters 2020年第6期31卷 1462-1473页

作者： Xiaoru Pan Jiahui Ji Nana Zhang mingyang xing Department of Chemistry and Chemical Engineering Weifang UniversityWeifang 261061China Key Laboratory for Advanced Materials and Institute of Fine Chemicals East China University of Science and TechnologyShanghai 200237China

Graphene is a two-dimensional nanomaterial with huge surface area,high carrier mobility and high mechanical *** of its great potential in nanotechnology and environmental protection,it has attracted much attention in environmental and energy fields since its discovery in *** graphene is a star material,many reviews have introduced its use in terms of energy,the research progress in the field of environment,especially water pollution control,has been rarely ***,we review exhaustively the research progress of graphene-based materials in environmental pollution remediation in the past ten ***,the advantages and classification of graphene were ***,the research progress and main achievements of graphene and its composites in the fields of photocatalytic degradation,pollutant adsorption and water treatment were emphatically described,and the mechanism of action in the above fields was ***,we discuss the problems existing in the preparation and summarize the application of graphene in the environment.

关键词： Graphene Nanomaterial Photocatalytic degradation Pollutant adsorption Water treatment

Efficient Fe（Ⅲ）/Fe（Ⅱ） cycling triggered by MoO2 in Fenton reaction for the degradation of dye molecules and the reduction of Cr（Ⅵ）

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Chinese Chemical Letters 2019年第12期30卷 2205-2210页

作者： Bin Shen Chencheng Dong Jiahui Ji mingyang xing Jinlong Zhang Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research Center School of Chemistry and Molecular Engineering East China University of Science and Technology

There is a relatively low efficiency of Fe(Ⅲ)/Fe(Ⅱ) conversion cycle and H2 O2 decomposition(<30%) in conventional Fenton process,which further results in a low production efficiency of ·OH and seriously restricts the application of ***,we report that the commercial MoO2 can be used as the cocatalyst in Fenton process to dramatically accelerate the oxidation of Lissamine rhodamine B(L-RhB),where the efficiency of Fe(Ⅲ)/Fe(Ⅱ) cycling is greatly enhanced in the Fenton reaction *** the L-RhB solution could be degraded nearly 100% in 1 min in the MoO2 cocatalytic Fenton system under the optimal reaction condition,which is apparently better than that of the conventional Fenton system(~50%).Different from the conventional Fenton reaction where the ’OH plays an important role in the oxidation process,it shows that 1 O2 contributes most in the MoO2 cocatalytic Fenton ***,it is found that the exposed Mo^4+ active sites on the surface of MoO2 powders can greatly promote the rate-limiting step of Fe^3+/Fe^2+ cycle conversion,thus minimizing the dosage of H2 O2(0.400 mmol/L) and Fe^2+(0.105 mmol/L).Interestingly,the MoO2 cocatalytic Fenton system also exhibits a good ability for reducing Cr(Ⅵ) ions,where the reduction ability for Cr(Ⅵ) reaches almost 100% within 2 *** short,this work shows a new discovery for M002 cocatalytic advanced oxidation processes(AOPs),which devotes a lot to the practical water remediation application.

关键词： Fenton reaction Co-catalytic Molybdenum dioxide Fe^3+/Fe^2+conversion Dye wastewater

Research progress of photocatalysis based on highly dispersed titanium in mesoporous SiO_2

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Chinese Chemical Letters 2019年第4期30卷 853-862页

作者： Chencheng Dong Jiahui Ji Zhe Yang Yifei Xiao mingyang xing Jinlong Zhang Key Laboratory for Advanced Materials and Institute of Fine Chemicals School of Chemistry & Molecular Engineering East China University of Science and Technology Department of Civil Engineering The University of Hong Kong

With the development of the human economy and green chemistry, people pay much more attention to environmental safety. Correspondingly, mesoporous TiO_2 and its correlated photocatalysts are able to help people seek for better life. In this review, first of all, we briefly introduce the preparations and applications of mesoporous TiO_2-SiO_2 materials, which exhibit excellent performance in pollutants decomposition and H_2 evolution in photocatalysis. Then, we review the mesoporous composites of TiSiO_2 materials, which are ideal materials used in the photoreduction of air pollutants such as CO_2, NO and NO_2. It is powerfully evident from the literature surveys that these TiO_2 based mesoporous photocatalysts possess a large potential in environment and energy development.

关键词： Mesoporous TiO2-SiO2 Ti-SiO2 Photocatalysis Photo-degradation Water splitting CO2 reduction

Regulating Lewis Acid-Base Sites over Fenton System for Enhancing Degradation of Pollutants in Saline and Buffered Wastewater

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Chinese Journal of Chemistry 2024年第21期42卷 2563-2571页

作者： Zhuan Chen Jun Li Bo Yang Jiazhen Cao Lingli Zhu mingyang xing Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science and Technology130 Meilong RoadShanghai200237 China School of Chemical Engineering The University of AdelaideAdelaideSA5005 Australia Shanghai Engineering Research Center for Multimedia Environmental Catalysis and Resource Utilization East China University of Science and Technology130 Meilong RoadShanghai200237 China

The saline and buffered environment in actual wastewater imposes higher demands on Fenton and Fenton-like catalytic *** study developed a MoS_(2)co-catalytic Fe_(2)O_(3)Fenton-like system with controllable Lewis acid-base sites,achieving efficient treatment of various model pollutants and actual industrial wastewater under neutral buffered *** acidic microenvironment structured by the edge S sites(Lewis basic sites)in the MoS_(2)/Fe_(2)O_(3)catalyst is susceptible to the influence of Lewis acidic sites constructed by Mo and Fe element,affecting catalytic *** the ratio of precursor amounts ensures the stable presence of the acidic microenvironment on the surface of catalyst,enabling the beneficial co-catalytic effect of Mo sites to be ***,it transcends the rigid constraints imposed by the Fenton reaction on reaction environments,thereby expanding the applicability of commonplace oxides such as Fe_(2)O_(3)in actual industrial water remediation.

关键词： Fenton MoS_(2) Fe_(2)O_(3) Lewis acid-base sites Acidicmicroenvironment Iron cycle Degradation/Wastewater

Sustainable activation of peroxymonosulfate by the Mo(Ⅳ)in MoS_(2) for the remediation of aromatic organic pollutants

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Chinese Chemical Letters 2020年第10期31卷 2803-2808页

作者： Mengmeng Du Qiuying Yi Jiahui Ji Qiaohong Zhu Huan Duan mingyang xing Jinlong Zhang Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Key Laboratory for Advanced Materials and Institute of Fine ChemicalsSchool of Chemistry&Molecular EngineeringEast China University of Science&TechnologyShanghai 200237China School of Chemistry and Chemical Engineering Southwest UniversityChongqing 400715China

Although MoS_(2) has been proved to be a very ideal cocatalyst in advanced oxidation process(AOPs),the activation process of peroxy mono sulfate(PMS)is still inseparable from metal ions which inevitably brings the risk of secondary pollution and it is not conducive to large-scale industrial *** this study,the commercial MoS_(2),as a durable and efficient catalyst,was used for directly activating PMS to degrade aromatic organic *** commercial MoS_(2)/PMS catalytic system demonstrated excellent removal efficiency of phenol and the total organic carbon(TOC)residual rate reach to 25%.The degradation rate was significantly reduced if the used MoS_(2) was directly carried out the next cycle experiment without any ***,the commercial MoS_(2) after post-treated with H2 O_(2) can exhibit good stability and recyclability for cyclic degradation of ***,the mechanism for the activation of PMS had been investigated by density functional theory(DFT)*** renewable Mo4+exposed on the surface of MoS_(2) was deduced as the primary active site,which realized the direct activation of PMS and avoided secondary *** into account the reaction cost and efficient activity,the development of commercial MoS_(2) catalytic system is expected to be applied in industrial wastewater.

关键词： Peroxymoosulfate Molybdenum disulfide Surface reaction Recyclability Sulfur vacancies Density functional theory

Defect electrons accelerate iron cycle of novel Fe-based Fenton:Long-term effective quinoline degradation

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Chinese Chemical Letters 2023年第6期34卷 598-605页

作者： Weikang Hu Ming Yang Qingyun Yan Jiahui Ji Yan Bao Jinlong Zhang mingyang xing Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai 200237China

Heterogeneous Fenton has been widely used in the disposal of organic pollutants,however,slow regeneration of≡Fe(II)remains limitation for its practical application of long-term ***,we come up with a novel Fe-based heterogeneous Fenton catalyst named as FeS_(x)O_(y)-X(X is the ratio of ethylene glycol to N,N-dimethylformamide).With the help of the abundant defect electrons in Sulfur vacancies,≡Fe(Ⅱ)regeneration on the surface of FeS_(x)O_(y)-1:1 was accelerated,resulting in a stable proportion of≡Fe(Ⅱ)on the surface,which maintained continuously stable generation of hydroxyl radical(·OH)and singlet oxygen(^(1)O_(2)).Thus,without any organic reagents or cocatalysts,FeS_(x)O_(y)-1:1 based Fenton system achieved effective long-term degradation of 560 mg/L quinoline within only 7 days,which was evidently better than reported Fe S and SV-Fe S_(2)(SV:Sulfur vacancy).The system had excellent adaptability to water quality and the COD removal rate of biochemical wastewater was as high as 79.8%.

关键词： Fenton reaction Quinoline Defect electron Iron cycle Heterogeneous catalyst

"Small amount for multiple times" of H_(2)O_(2) feeding way in MoS_(2)-Fex heterogeneous fenton for enhancing sulfadiazine degradation

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Chinese Chemical Letters 2022年第3期33卷 1365-1372页

作者： Zhuan Chen Cheng Lian Kai Huang Jiahui Ji Qingyun Yan Jinlong Zhang mingyang xing Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai 200237China

In recent years, MoS_(2) catalyzed/cocatalyzed Fenton/Fenton-like systems have attracted wide attention in the field of pollution control, but there are few studies on the effect of H_(2)O_(2) feeding way on the whole Fenton process. Here, we report a new type of composite catalyst (MoS_(2)-Fe_(x)) prepared in a simple way with highly dispersed iron to provide more active sites. MoS_(2)-Fe_(x) was proved to possess selectivity for singlet oxygen (^(1)O_(2)) in effectively degrading sulfadiazine with a wide pH adaptability (4.0~10.0). Importantly, the mechanism of the interaction between H_(2)O_(2) and MoS_(2) on the Fenton reaction activity was revealed through the combination of experiment and density functional theory (DFT) calculations. Compared to the traditional “a large amount for one time” feeding way of H_(2)O_(2), the “small amount for multiple times” of H_(2)O_(2) feeding way can increase the degradation rate of sulfadiazine from 36.9% to 91.1% in the MoS_(2)-Fe_(x) heterogeneous Fenton system. It is demonstrated that the “small amount for multiple times” of H_(2)O_(2) feeding way can reduce the side reaction of decomposition of H_(2)O_(2) by MoS_(2) and effectively improve the utilization rate of H_(2)O_(2) and the stability of MoS_(2)-Fe_(x). Compared with Fe_(2)O_(3)^(-)based Fenton system, MoS_(2)-Fe_(x) can significantly save the amount of H_(2)O_(2). Compared with nano-iron powder, the formation of iron sludge in MoS_(2)-Fe_(x) system was significantly reduced. Furthermore, long-term degradation test showed that the MoS_(2)-Fe75/H_(2)O_(2) system could maintain the effectiveness of degrading organic pollutants for 10 days (or even longer). This study has a guiding significance for the large-scale treatment of industrial wastewater by improved Fenton technology in the future.

关键词： Fenton reaction Co-catalytic Molybdenum sulfide Hydrogen peroxide Singlet oxygen

Graphene-Based Photo-Fenton Catalysts for Pollutant Control

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Transactions of Tianjin University 2021年第2期27卷 110-126页

作者： Yan Bao Qingyun Yan Jiahui Ji Bocheng Qiu Jinlong Zhang mingyang xing Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Jiangsu Key Laboratory of Pesticide Sciences Department of ChemistryCollege of SciencesNanjing Agricultural UniversityNanjing 210095China

Water pollution is a global environmental issue with multi-dimensional infl uences on human *** strategies,such as photo-Fenton reaction,have been employed to remove recalcitrant ***-dimensional(2D)graphene and its threedimensional(3D)confi gurations have attracted considerable attention as emerging carbon-based catalysts in photo-Fenton fi elds owing to their alluring properties in electron transfer,reactant adsorption,and light *** review summarizes the recent developments in 2D and 3D graphene-based catalysts for photo-Fenton *** structures,characteristics,activity,and mechanisms are *** conclusions and outlooks are proposed for the profound understanding of challenges and future directions.

关键词： Photo-Fenton Graphene Pollutant control Aerogel Hydrogel

Gold-loaded graphene oxide/PDPB composites for the synchronous removal of Cr(Ⅵ) and phenol

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Chinese Journal of Catalysis 2018年第1期39卷 8-15页

作者： Jun Liu Wenzhang Fang Yuhang Wang mingyang xing mingyang xing Key Laboratory for Advanced Materials and Institute of Fine Chemicals School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 China

The construction of novel inorganic‐organic hybrid nanomaterials for synchronous photocatalyticremoval of heavy metal ions and organic pollutants has received significant *** successfullysynthesized gold‐loaded graphene oxide/PDPB(polymer poly(diphenylbutadiyne))composites(Au‐GO/PDPB)through a facile mechanical agitation and photoreduction *** compositeswere characterized by XPS and TEM images,which confirmed the presence of GO and Au nanoparticleson the *** as‐prepared Au‐GO/PDPB composites displayed enhanced photocatalytic activity compared with that of pure PDPB for the synchronous photoreduction of hexavalent chromium(Cr(VI))and photo‐oxidation of *** also determined the optimal loading mass of GO and Au nanoparticles on the PDPB;the Au1‐GO2/PDPB(2.0wt%GO and1.0wt%Au)composite displayed the best photocatalytic activity among all the *** study provides a facile way to prepare inorganic‐organic composites for the synchronous photocatalytic removal of heavy metal ions and organic pollutants.?2018,Dalian Institute of Chemical Physics,Chinese Academy of *** by Elsevier *** rights reserved.

关键词： Photocatalysis Heavy metal ion Organic pollutant Polymer poly(diphenylbutadiyne) Synchronous removal