Degradation of cellulose to chemicals is one of major routes for biomass conversion. Here, a new simple and two-step method has been developed to convert cellulose in its homogeneously alkaline solution to organic aci...Degradation of cellulose to chemicals is one of major routes for biomass conversion. Here, a new simple and two-step method has been developed to convert cellulose in its homogeneously alkaline solution to organic acids under atmospheric pressure at mild temperature. At first, cellulose was degraded to smM1 molecular intermediates at 110 ℃ for 3 h under atmospheric pressure, and then it was oxidized with H202 at 50 ℃ for 4 h. Under the optimal condition, 73.5% conversion of cellulose could be achieved, and the yield of organic acids was 32.8% (formic acid), 11.6% (lactic acid), and 2.3% (oxalic acid), respectively. It is noteworthy that the new strategy reduces energy consumption in the process of reaction, unlike the hydrothermal reaction under high temperature and high pressure.展开更多
A polytetrafluoroethylene (PTFE)-doped PbO2 electrode on a Ti substrate was prepared by galvanostatic method from the sulfamic acid bath (Ti/PTFE-F-PbO2-I) or nitric acid bath (Ti/PTFE-F-PbO2-II). Scanning Elect...A polytetrafluoroethylene (PTFE)-doped PbO2 electrode on a Ti substrate was prepared by galvanostatic method from the sulfamic acid bath (Ti/PTFE-F-PbO2-I) or nitric acid bath (Ti/PTFE-F-PbO2-II). Scanning Electron Microscopy revealed that the Ti/PTFE-PbO2-I electrode had a more regular morphology with smaller size crystals than the Ti/PTFE-F-PbO2-II electrode. On the basis of the results of both the accelerated electrolysis test and the empirical formula for estimating the service life of an electrode, the service life of the Ti/PTFE-PbO2-I electrode was predicted to be more than 7 years under conventional electrolysis conditions (0.1 A·cm^-2). During the treatment of 4-chlorophenol-contaminated water, the Ti/PTFE-PbO2-I anode showed both a good electro-catalytic activity and high electrochemical stability, exhibiting an excellent potential application.展开更多
An environmentally friendly Mn‐oxide‐supported metal‐organic framework(MOF),Mn3O4/ZIF‐8,was successfully prepared using a facile solvothermal method,with a formation mechanism proposed.The composite was characteri...An environmentally friendly Mn‐oxide‐supported metal‐organic framework(MOF),Mn3O4/ZIF‐8,was successfully prepared using a facile solvothermal method,with a formation mechanism proposed.The composite was characterized using X‐ray diffraction,scanning electron microscopy,transmission electron microscopy,X‐ray photoelectron microscopy,and Fourier‐transform infrared spectroscopy.After characterization,the MOF was used to activate peroxymonosulfate(PMS)for degradation of the refractory pollutant rhodamine B(RhB)in water.The composite prepared at a0.5:1mass ratio of Mn3O4to ZIF‐8possessed the highest catalytic activity with negligible Mn leaching.The maximum RhB degradation of approximately98%was achieved at0.4g/L0.5‐Mn/ZIF‐120,0.3g/L PMS,and10mg/L initial RhB concentration at a reaction temperature of23°C.The RhB degradation followed first‐order kinetics and was accelerated with increased0.5‐Mn/ZIF‐120and PMS dosages,decreased initial RhB concentration,and increased reaction temperature.Moreover,quenching tests indicated that?OH was the predominant radical involved in the RhB degradation;the?OH mainly originated from SO4??and,hence,PMS.Mn3O4/ZIF‐8also displayed good reusability for RhB degradation in the presence of PMS over five runs,with a RhB degradation efficiency of more than96%and Mn leaching of less than5%for each run.Based on these findings,a RhB degradation mechanism was proposed.展开更多
The factors and mechanisms of oxidative degradation of three organophosphorus pesticides (dichlorvos, methamidophos and phoxim) were studied with sodium percarbonate (SPC) as a solid oxidant. The result showed tha...The factors and mechanisms of oxidative degradation of three organophosphorus pesticides (dichlorvos, methamidophos and phoxim) were studied with sodium percarbonate (SPC) as a solid oxidant. The result showed that SPC has highly activity in degrading these organophosphous pesticides. The most efficient degradation of pesticides occurred under basic conditions and the degradation rates increased with time extension and high temperature. The degradation of organophosphorus pesticides was expected to get even better results at lower initial concentration. Furthermore, we analyzed the intermediate products by NMP, spectrometry. On the basis of the analytical result, the oxidative degradation mechanism was proposed for each organophosphous pesticide. It is significant to understand the environment chemistry of organophosphorus pesticides in environmental system.展开更多
Recent world events have emphasized the need to develop innovative, functional materials that will safely neutralize chemical warfare (CW) agents in situ to protect military personnel and civilians from dermal expos...Recent world events have emphasized the need to develop innovative, functional materials that will safely neutralize chemical warfare (CW) agents in situ to protect military personnel and civilians from dermal exposure. Here, we demonstrate the efficacy of a novel, proof-of-concept design for a Cu-containing catalyst, chemically bonded to a single-wall carbon nanotube (SWCNT) structural support, to effectively degrade an organophosphate simulant. SWCNTs have high tensile strength and are flexible and light-weight, which make them a desirable structural component for unique, fabric-like materials. This study aims to develop a self-decontaminating, carbon nanotube-derived material that can ultimately be incorporated into a wearable fabric or protective material to minimize dermal exposure to organophosphate nerve agents and to prevent accidental exposure during decontamination procedures. Carboxylated SWCNTs were functionalized with a polymer, which contained Cu-chelating bipyridine groups, and their catalytic activity against an organophosphate simulant was measured over time. The catalytically active, functionalized nanomaterial was characterized using X-ray fluorescence and Raman spectroscopy. Assuming zeroth-order reaction kinetics, the hydrolysis rate of the organophosphate simulant, as monitored by UV-vis absorption in the presence of the catalytically active nanomaterial, was 63 times faster than the uncatalyzed hydrolysis rate for a sample containing only carboxylated SWCNTs or a control sample containing no added nanotube materials.展开更多
基金This work was supported by the National Natural Science Foundation of China (No.51373162), and the Natural Science Foundation of Anhui Province (No.1408085MKL03).
文摘Degradation of cellulose to chemicals is one of major routes for biomass conversion. Here, a new simple and two-step method has been developed to convert cellulose in its homogeneously alkaline solution to organic acids under atmospheric pressure at mild temperature. At first, cellulose was degraded to smM1 molecular intermediates at 110 ℃ for 3 h under atmospheric pressure, and then it was oxidized with H202 at 50 ℃ for 4 h. Under the optimal condition, 73.5% conversion of cellulose could be achieved, and the yield of organic acids was 32.8% (formic acid), 11.6% (lactic acid), and 2.3% (oxalic acid), respectively. It is noteworthy that the new strategy reduces energy consumption in the process of reaction, unlike the hydrothermal reaction under high temperature and high pressure.
基金Supported by the National Natural Science Foundation of China (20406019, 20876151)
文摘A polytetrafluoroethylene (PTFE)-doped PbO2 electrode on a Ti substrate was prepared by galvanostatic method from the sulfamic acid bath (Ti/PTFE-F-PbO2-I) or nitric acid bath (Ti/PTFE-F-PbO2-II). Scanning Electron Microscopy revealed that the Ti/PTFE-PbO2-I electrode had a more regular morphology with smaller size crystals than the Ti/PTFE-F-PbO2-II electrode. On the basis of the results of both the accelerated electrolysis test and the empirical formula for estimating the service life of an electrode, the service life of the Ti/PTFE-PbO2-I electrode was predicted to be more than 7 years under conventional electrolysis conditions (0.1 A·cm^-2). During the treatment of 4-chlorophenol-contaminated water, the Ti/PTFE-PbO2-I anode showed both a good electro-catalytic activity and high electrochemical stability, exhibiting an excellent potential application.
基金supported by the National Key Research and Development Program of China (2016YFB0700504)~~
文摘An environmentally friendly Mn‐oxide‐supported metal‐organic framework(MOF),Mn3O4/ZIF‐8,was successfully prepared using a facile solvothermal method,with a formation mechanism proposed.The composite was characterized using X‐ray diffraction,scanning electron microscopy,transmission electron microscopy,X‐ray photoelectron microscopy,and Fourier‐transform infrared spectroscopy.After characterization,the MOF was used to activate peroxymonosulfate(PMS)for degradation of the refractory pollutant rhodamine B(RhB)in water.The composite prepared at a0.5:1mass ratio of Mn3O4to ZIF‐8possessed the highest catalytic activity with negligible Mn leaching.The maximum RhB degradation of approximately98%was achieved at0.4g/L0.5‐Mn/ZIF‐120,0.3g/L PMS,and10mg/L initial RhB concentration at a reaction temperature of23°C.The RhB degradation followed first‐order kinetics and was accelerated with increased0.5‐Mn/ZIF‐120and PMS dosages,decreased initial RhB concentration,and increased reaction temperature.Moreover,quenching tests indicated that?OH was the predominant radical involved in the RhB degradation;the?OH mainly originated from SO4??and,hence,PMS.Mn3O4/ZIF‐8also displayed good reusability for RhB degradation in the presence of PMS over five runs,with a RhB degradation efficiency of more than96%and Mn leaching of less than5%for each run.Based on these findings,a RhB degradation mechanism was proposed.
文摘The factors and mechanisms of oxidative degradation of three organophosphorus pesticides (dichlorvos, methamidophos and phoxim) were studied with sodium percarbonate (SPC) as a solid oxidant. The result showed that SPC has highly activity in degrading these organophosphous pesticides. The most efficient degradation of pesticides occurred under basic conditions and the degradation rates increased with time extension and high temperature. The degradation of organophosphorus pesticides was expected to get even better results at lower initial concentration. Furthermore, we analyzed the intermediate products by NMP, spectrometry. On the basis of the analytical result, the oxidative degradation mechanism was proposed for each organophosphous pesticide. It is significant to understand the environment chemistry of organophosphorus pesticides in environmental system.
文摘Recent world events have emphasized the need to develop innovative, functional materials that will safely neutralize chemical warfare (CW) agents in situ to protect military personnel and civilians from dermal exposure. Here, we demonstrate the efficacy of a novel, proof-of-concept design for a Cu-containing catalyst, chemically bonded to a single-wall carbon nanotube (SWCNT) structural support, to effectively degrade an organophosphate simulant. SWCNTs have high tensile strength and are flexible and light-weight, which make them a desirable structural component for unique, fabric-like materials. This study aims to develop a self-decontaminating, carbon nanotube-derived material that can ultimately be incorporated into a wearable fabric or protective material to minimize dermal exposure to organophosphate nerve agents and to prevent accidental exposure during decontamination procedures. Carboxylated SWCNTs were functionalized with a polymer, which contained Cu-chelating bipyridine groups, and their catalytic activity against an organophosphate simulant was measured over time. The catalytically active, functionalized nanomaterial was characterized using X-ray fluorescence and Raman spectroscopy. Assuming zeroth-order reaction kinetics, the hydrolysis rate of the organophosphate simulant, as monitored by UV-vis absorption in the presence of the catalytically active nanomaterial, was 63 times faster than the uncatalyzed hydrolysis rate for a sample containing only carboxylated SWCNTs or a control sample containing no added nanotube materials.