Micro-scale Al-Zn-Mg/Fe composite powders (MAF) with high reactivity and good storage properties were prepared by reducing iron onto the surface of Al-Zn-Mg alloy powders. Experimental results show that MAF as advance...Micro-scale Al-Zn-Mg/Fe composite powders (MAF) with high reactivity and good storage properties were prepared by reducing iron onto the surface of Al-Zn-Mg alloy powders. Experimental results show that MAF as advanced zero-valent iron are highly effective for degradation of chlorinated organic compounds. The efficiency of degradation for carbon tetrachloride and perchloroethylene is higher than 99% within a period of 2 h. The efficiency of degradation for trichloroethylene by MAF after storing for one month is equivalent to that by freshly prepared nano-size zero-valent iron particles.展开更多
Chlorinated organic compounds are emerging pollutants of widespread concern because of their toxicity,bioaccumulation,persistence,and lack of adequate regulatory measures.Their abiotic transformation,facilitated by ir...Chlorinated organic compounds are emerging pollutants of widespread concern because of their toxicity,bioaccumulation,persistence,and lack of adequate regulatory measures.Their abiotic transformation,facilitated by iron-bearing minerals,is critical to their natural dissipation in soils and sediments.However,further exploration is needed to understand their underlying mechanisms and potential engineering applications under different redox conditions.This paper reviews the abiotic transformation behaviors and mechanisms of chlorinated organics at the active surface of iron-bearing minerals under anoxic and oxic conditions and summarizes the strategies for enhancing the abiotic transformation efficiency of chlorinated organics.The abiotic transformation rate under oxic conditions can be a few orders of magnitude higher than that under anoxic conditions.Under anoxic conditions,chlorinated organics undergo reductive dechlorination through reductive elimination,hydrogenolysis,dehydrohalogenation,and nucleophilic substitution.A close relationship between the abiotic transformation of chlorinated organics and the production of hydroxyl radicals by iron-bearing minerals under oxic conditions was discovered.Synthetic active iron-bearing minerals,carbonaceous materials,and biological synergy can facilitate abiotic dechlorination under anoxic conditions.Meanwhile,the regulation of redox conditions,the introduction of ligands,and the utilization of coexisting anions are proposed to enhance oxidative degradation.This study is expected to improve the comprehension of the abiotic degradation of chlorinated organics mediated by iron-bearing minerals and provide the theoretical foundation for developing new approaches aimed at addressing chlorinated organic pollution.展开更多
Electrochemical dechlorination reaction(EDR)is a promising,environmentally friendly,and economically profitable technology for treating chlorinated organic pollutants.For efficient environmental protection,electrocata...Electrochemical dechlorination reaction(EDR)is a promising,environmentally friendly,and economically profitable technology for treating chlorinated organic pollutants.For efficient environmental protection,electrocatalysts with high stability and low cost are of extremely significance to the development of EDR technology.Carbon-based materials have aroused broad interest as electrocatalysts for many electrochemical reactions due to their characteristics including large specific surface area,controllable structure,good conductivity,and chemical stability.For EDR,the carbon-based materials also show many unique superiorities,like strong adsorption capacity to chlorinated organic compounds(COCs),excellent catalytic activity and stability,and environmental compatibility.This review starts with a detailed summary on the mechanisms of electrochemical dechlorination(direct and indirect electron transfer pathway)and factors affecting the effectiveness of EDR.Then the paper comprehensively overviews the current progresses of carbon-based materials for EDR of COCs,following their two major application scenarios,i.e.,directly as electrocatalysts and as advanced supports for other catalysts.Moreover,the formation of different active sites in carbon-based electrocatalysts and their EDR activities are analyzed.Finally,the current challenges and perspectives in this field are discussed.This review will provide an in-depth understanding for the design of advanced carbon-based materials and promote the development of EDR technology.展开更多
High-surface-area mesoprous powders of γ-Al2O3 doped with Cu^2+, Cr^3+, and V^3+ ions were prepared uia a modified sol-gel method and were investigated as catalysts for the oxidation of chlorinated organic compoun...High-surface-area mesoprous powders of γ-Al2O3 doped with Cu^2+, Cr^3+, and V^3+ ions were prepared uia a modified sol-gel method and were investigated as catalysts for the oxidation of chlorinated organic compounds. The composites retained high surface areas and pore volumes comparable with those of undoped γ-Al2O3 and the presence of the transition metal ions enhanced their surface acidic properties. The catalytic activity of the prepared catalysts in the oxidation of 1,2-dichloroethane (DCE) was studied in the temperature range of 250-400℃. The catalytic activity and product selectivity were strongly dependent on the presence and the type of dopant ion. While Cu^2+- and Cr^3+-containing catalysts showed 100% conversion at 300℃ and 350℃, V3+-containing catalyst showed considerably lower conversion. Furthermore, while the major products of the reactions over γ-alumina were vinyl chloride (C2H3Cl) and hydrogen chloride (HCl) at all temperatures, Cu- and Cr-doped catalysts showed siguiticantly stronger capability for deep oxidation to CO2.展开更多
文摘Micro-scale Al-Zn-Mg/Fe composite powders (MAF) with high reactivity and good storage properties were prepared by reducing iron onto the surface of Al-Zn-Mg alloy powders. Experimental results show that MAF as advanced zero-valent iron are highly effective for degradation of chlorinated organic compounds. The efficiency of degradation for carbon tetrachloride and perchloroethylene is higher than 99% within a period of 2 h. The efficiency of degradation for trichloroethylene by MAF after storing for one month is equivalent to that by freshly prepared nano-size zero-valent iron particles.
基金supported by the National Natural Science Foundation of China(Grant No.52100180)the Fundamental Research Funds for the Central Universities(Grant No.531118010817).
文摘Chlorinated organic compounds are emerging pollutants of widespread concern because of their toxicity,bioaccumulation,persistence,and lack of adequate regulatory measures.Their abiotic transformation,facilitated by iron-bearing minerals,is critical to their natural dissipation in soils and sediments.However,further exploration is needed to understand their underlying mechanisms and potential engineering applications under different redox conditions.This paper reviews the abiotic transformation behaviors and mechanisms of chlorinated organics at the active surface of iron-bearing minerals under anoxic and oxic conditions and summarizes the strategies for enhancing the abiotic transformation efficiency of chlorinated organics.The abiotic transformation rate under oxic conditions can be a few orders of magnitude higher than that under anoxic conditions.Under anoxic conditions,chlorinated organics undergo reductive dechlorination through reductive elimination,hydrogenolysis,dehydrohalogenation,and nucleophilic substitution.A close relationship between the abiotic transformation of chlorinated organics and the production of hydroxyl radicals by iron-bearing minerals under oxic conditions was discovered.Synthetic active iron-bearing minerals,carbonaceous materials,and biological synergy can facilitate abiotic dechlorination under anoxic conditions.Meanwhile,the regulation of redox conditions,the introduction of ligands,and the utilization of coexisting anions are proposed to enhance oxidative degradation.This study is expected to improve the comprehension of the abiotic degradation of chlorinated organics mediated by iron-bearing minerals and provide the theoretical foundation for developing new approaches aimed at addressing chlorinated organic pollution.
基金supported by the 2021 Hong Kong Scholars Program(No.XJ2021005)the National Natural Science Foundation of China(Nos.52301261,52372229,and 52172241)+2 种基金the General Research Fund of Hong Kong(Nos.CityU 11308321 and CityU 11315622)the Green Tech Fund(No.GTF202220105)the City University of Hong Kong(No.9020002).
文摘Electrochemical dechlorination reaction(EDR)is a promising,environmentally friendly,and economically profitable technology for treating chlorinated organic pollutants.For efficient environmental protection,electrocatalysts with high stability and low cost are of extremely significance to the development of EDR technology.Carbon-based materials have aroused broad interest as electrocatalysts for many electrochemical reactions due to their characteristics including large specific surface area,controllable structure,good conductivity,and chemical stability.For EDR,the carbon-based materials also show many unique superiorities,like strong adsorption capacity to chlorinated organic compounds(COCs),excellent catalytic activity and stability,and environmental compatibility.This review starts with a detailed summary on the mechanisms of electrochemical dechlorination(direct and indirect electron transfer pathway)and factors affecting the effectiveness of EDR.Then the paper comprehensively overviews the current progresses of carbon-based materials for EDR of COCs,following their two major application scenarios,i.e.,directly as electrocatalysts and as advanced supports for other catalysts.Moreover,the formation of different active sites in carbon-based electrocatalysts and their EDR activities are analyzed.Finally,the current challenges and perspectives in this field are discussed.This review will provide an in-depth understanding for the design of advanced carbon-based materials and promote the development of EDR technology.
基金United Arab Emirates University through NRF grant, 2011
文摘High-surface-area mesoprous powders of γ-Al2O3 doped with Cu^2+, Cr^3+, and V^3+ ions were prepared uia a modified sol-gel method and were investigated as catalysts for the oxidation of chlorinated organic compounds. The composites retained high surface areas and pore volumes comparable with those of undoped γ-Al2O3 and the presence of the transition metal ions enhanced their surface acidic properties. The catalytic activity of the prepared catalysts in the oxidation of 1,2-dichloroethane (DCE) was studied in the temperature range of 250-400℃. The catalytic activity and product selectivity were strongly dependent on the presence and the type of dopant ion. While Cu^2+- and Cr^3+-containing catalysts showed 100% conversion at 300℃ and 350℃, V3+-containing catalyst showed considerably lower conversion. Furthermore, while the major products of the reactions over γ-alumina were vinyl chloride (C2H3Cl) and hydrogen chloride (HCl) at all temperatures, Cu- and Cr-doped catalysts showed siguiticantly stronger capability for deep oxidation to CO2.