The Electro-Fenton(EF)process is one of the promising advanced oxidation processes(AOPs)for environmental remediation.The H_(2)O_(2) yield of EF process largely determines its performance on organic pollutants degrada...The Electro-Fenton(EF)process is one of the promising advanced oxidation processes(AOPs)for environmental remediation.The H_(2)O_(2) yield of EF process largely determines its performance on organic pollutants degradation.Conventional Pd-catalytic EF process generates H_(2)O_(2) via the combination reaction of anodic O_(2) and cathodic H;.However,the relatively expensive catalyst limits its application.Herein,a hybrid Pd/activated carbon(Pd/AC)-stainless steel mesh(SS)cathode(PACSS)was proposed,which enables more efficie nt H_(2)O_(2)generation.It utilizes AC,the support of Pd catalyst,as part of cathode for H_(2)O_(2) generation via 2-electron anodic O_(2) reduction,and SS serve as a current distributor.Moreover,H_(2)O_(2) could be catalytically decomposed upon AC to generate highly reactive·OH,which avoids the use of Fe;.Compared with conventional Pd catalyst,H_(2)O_(2) concentration obtained by PACSS cathode is248.2%higher,the O_(2)utilization efficiency was also increased from 3.2%to 10.8%.Within 50 min,26.3%,72.5%,and 94.0%H_(2)O_(2) was decomposed by Pd,AC,and Pd/AC.Fluorescence detection results implied that Pd/AC is effective upon H_(2)O_(2) activation for·OH generation.Finally,iron-free EF process enabled by PACSS cathode was examined to be effective for reactive blue 19(RB19)degradation.After continuous running for 10 cycles(500 min),the PACSS cathode was still stable for H_(2)O_(2)generation,H_(2)O_(2)activation,and RB19 degradation,showing its potential application for organic pollutants degradation without increase in the running cost.展开更多
Restraining the shuttle effects of lithium polysulfides is the key to improve the cycling reversibility and stability of lithium-sulfur(Li-S)batteries for which design of robust sulfur hosts has been regarded as the m...Restraining the shuttle effects of lithium polysulfides is the key to improve the cycling reversibility and stability of lithium-sulfur(Li-S)batteries for which design of robust sulfur hosts has been regarded as the most effective strategy.In this work,we report a new type of hybrid sulfur host which is composed of Al_(2)O_(3) homogenously decorated in nitrogen-rich mesoporous carbon framework(NMC-Al_(2)O_(3)).The NMC-Al_(2)O_(3) hybrid host features a poly-dispersed spherical morphology and a mesoporous configuration with high surface area and large pore volume that can accommodate a high sulfur content up to 73.5 wt.%.As a result,the fabricated NMC-Al_(2)O_(3)-S cathode exhibits all-round improvements in electrochemical properties in term of capacities(1,212 mAh·g^(-1)at 0.2 C;755 mAh·g^(-1)at 2 C),cycling charge-discharge reversibility(sustainably 100%efficiencies)and stability(1,000 cycles with only 0.023%capacity decay per cycle at 0.5 C).By contrast,the Al_(2)O_(3)-free NMC-S cathode shows both decreased capacities and rapidly descending Coulombic efficiencies during cycling.Density functional theory(DFH")calculations further reveal that the implanted Al_(2)O_(3) can greatly enhance the chemical adsorption and catalytic conversion for various lithium polysulfides and thereby effectively prevent the polysulfide shuttling and significantly improve the utilizability,reversibility and stability of sulfur cathode.展开更多
A simple method was developed to tune the porosity of coal-derived activated carbons,which provided a model adsorbent system to investigate the volumetric CO_(2)adsorption performance.Specifically,the method involved ...A simple method was developed to tune the porosity of coal-derived activated carbons,which provided a model adsorbent system to investigate the volumetric CO_(2)adsorption performance.Specifically,the method involved the variation of the activation temperature in a K2CO3 induced chemical activation process which could yield activated carbons with defined microporous(<2 nm,including ultra-microporous<1 nm)and meso-microporous structures.CO_(2)adsorption isotherms revealed that the microporous activated carbon has the highest measured CO_(2)adsorption capacity(6.0 mmol∙g^(–1)at 0℃and 4.1 mmol∙g^(-1)at 25℃),whilst ultra-microporous activated carbon with a high packing density exhibited the highest normalized capacity with respect to packing volume(1.8 mmol∙cm−3 at 0℃and 1.3 mmol∙cm^(–3)at 25℃),which is significant.Both experimental correlation analysis and molecular dynamics simulation demonstrated that(i)volumetric CO_(2)adsorption capacity is directly proportional to the ultra-micropore volume,and(ii)an increase in micropore sizes is beneficial to improve the volumetric capacity,but may lead a low CO_(2)adsorption density and thus low pore space utilization efficiency.The adsorption experiments on the activated carbons established the criterion for designing CO_(2)adsorbents with high volumetric adsorption capacity.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.52006049,51776055)the China Postdoctoral Science Foundation(Nos.2019M661293,2020T130149)。
文摘The Electro-Fenton(EF)process is one of the promising advanced oxidation processes(AOPs)for environmental remediation.The H_(2)O_(2) yield of EF process largely determines its performance on organic pollutants degradation.Conventional Pd-catalytic EF process generates H_(2)O_(2) via the combination reaction of anodic O_(2) and cathodic H;.However,the relatively expensive catalyst limits its application.Herein,a hybrid Pd/activated carbon(Pd/AC)-stainless steel mesh(SS)cathode(PACSS)was proposed,which enables more efficie nt H_(2)O_(2)generation.It utilizes AC,the support of Pd catalyst,as part of cathode for H_(2)O_(2) generation via 2-electron anodic O_(2) reduction,and SS serve as a current distributor.Moreover,H_(2)O_(2) could be catalytically decomposed upon AC to generate highly reactive·OH,which avoids the use of Fe;.Compared with conventional Pd catalyst,H_(2)O_(2) concentration obtained by PACSS cathode is248.2%higher,the O_(2)utilization efficiency was also increased from 3.2%to 10.8%.Within 50 min,26.3%,72.5%,and 94.0%H_(2)O_(2) was decomposed by Pd,AC,and Pd/AC.Fluorescence detection results implied that Pd/AC is effective upon H_(2)O_(2) activation for·OH generation.Finally,iron-free EF process enabled by PACSS cathode was examined to be effective for reactive blue 19(RB19)degradation.After continuous running for 10 cycles(500 min),the PACSS cathode was still stable for H_(2)O_(2)generation,H_(2)O_(2)activation,and RB19 degradation,showing its potential application for organic pollutants degradation without increase in the running cost.
基金the Open Project of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering,Ningxia University(No.2018-13K)and the Fundamental Research Funds for the Central Universities.
文摘Restraining the shuttle effects of lithium polysulfides is the key to improve the cycling reversibility and stability of lithium-sulfur(Li-S)batteries for which design of robust sulfur hosts has been regarded as the most effective strategy.In this work,we report a new type of hybrid sulfur host which is composed of Al_(2)O_(3) homogenously decorated in nitrogen-rich mesoporous carbon framework(NMC-Al_(2)O_(3)).The NMC-Al_(2)O_(3) hybrid host features a poly-dispersed spherical morphology and a mesoporous configuration with high surface area and large pore volume that can accommodate a high sulfur content up to 73.5 wt.%.As a result,the fabricated NMC-Al_(2)O_(3)-S cathode exhibits all-round improvements in electrochemical properties in term of capacities(1,212 mAh·g^(-1)at 0.2 C;755 mAh·g^(-1)at 2 C),cycling charge-discharge reversibility(sustainably 100%efficiencies)and stability(1,000 cycles with only 0.023%capacity decay per cycle at 0.5 C).By contrast,the Al_(2)O_(3)-free NMC-S cathode shows both decreased capacities and rapidly descending Coulombic efficiencies during cycling.Density functional theory(DFH")calculations further reveal that the implanted Al_(2)O_(3) can greatly enhance the chemical adsorption and catalytic conversion for various lithium polysulfides and thereby effectively prevent the polysulfide shuttling and significantly improve the utilizability,reversibility and stability of sulfur cathode.
基金supported by the National Natural Science Foundation of China(Grant No.51806050)the Fundamental Research Funds for the Central Universities of Harbin Institute of Technology.
文摘A simple method was developed to tune the porosity of coal-derived activated carbons,which provided a model adsorbent system to investigate the volumetric CO_(2)adsorption performance.Specifically,the method involved the variation of the activation temperature in a K2CO3 induced chemical activation process which could yield activated carbons with defined microporous(<2 nm,including ultra-microporous<1 nm)and meso-microporous structures.CO_(2)adsorption isotherms revealed that the microporous activated carbon has the highest measured CO_(2)adsorption capacity(6.0 mmol∙g^(–1)at 0℃and 4.1 mmol∙g^(-1)at 25℃),whilst ultra-microporous activated carbon with a high packing density exhibited the highest normalized capacity with respect to packing volume(1.8 mmol∙cm−3 at 0℃and 1.3 mmol∙cm^(–3)at 25℃),which is significant.Both experimental correlation analysis and molecular dynamics simulation demonstrated that(i)volumetric CO_(2)adsorption capacity is directly proportional to the ultra-micropore volume,and(ii)an increase in micropore sizes is beneficial to improve the volumetric capacity,but may lead a low CO_(2)adsorption density and thus low pore space utilization efficiency.The adsorption experiments on the activated carbons established the criterion for designing CO_(2)adsorbents with high volumetric adsorption capacity.
