CaCl_(2)·6H_(2)O/expanded vermiculite shape stabilized phase change materials(CEV)was prepared by atmospheric impregnation method.Using gold mine tailings as aggregate of cemented paste backfill(CPB)material,the ...CaCl_(2)·6H_(2)O/expanded vermiculite shape stabilized phase change materials(CEV)was prepared by atmospheric impregnation method.Using gold mine tailings as aggregate of cemented paste backfill(CPB)material,the CPB with CEV added was prepared,and the specific heat capacity,thermal conductivity,and uniaxial compressive strength(UCS)of CPB with different cement-tailing ratios and CEV addition ratios were tested,the influence of the above variables on the thermal and mechanical properties of CPB was analyzed.The results show that the maximum encapsulation capacity of expanded vermiculite for CaCl_(2)·6H_(2)O is about 60%,and the melting and solidification enthalpies of CEV can reach 98.87 J/g and 97.56 J/g,respectively.For the CPB without CEV,the specific heat capacity,thermal conductivity,and UCS decrease with the decrease of cement-tailing ratio.For the CPB with CEV added,with the increase of CEV addition ratio,the specific heat capacity increases significantly,and the sensible heat storage capacity and latent heat storage capacity can be increased by at least 10.74%and 218.97%respectively after adding 12%CEV.However,the addition of CEV leads to the increase of pores,and the thermal conductivity and UCS both decrease with the increase of CEV addition.When cement-tailing ratio is 1:8 and 6%,9%,and 12%of CEV are added,the 28-days UCS of CPB is less than 1 MPa.Considering the heat storage capacity and cost price of backfill,the recommended proportion scheme of CPB material presents cement-tailing ratio of 1:6 and 12%CEV,and the most recommended heat storage/release temperature cycle range of CPB with added CEV is from 20 to 40℃.This work can provide theoretical basis for the utilization of heat storage backfill in green mines.展开更多
CO2和H2O气体浓度是农田小气候的2个重要指标,一般采用CO2/H2O分析仪进行测定,为减少人为干扰,需使用气管将待测区域气体传输至分析器,而气管的材质及其长度会影响CO2/H2O测定时读数稳定所需的时间。本研究采用8种常用材质的气管及5种...CO2和H2O气体浓度是农田小气候的2个重要指标,一般采用CO2/H2O分析仪进行测定,为减少人为干扰,需使用气管将待测区域气体传输至分析器,而气管的材质及其长度会影响CO2/H2O测定时读数稳定所需的时间。本研究采用8种常用材质的气管及5种气管长度进行双因素随机区组试验,以筛选CO2/H2O测定所需的最佳气管材质及长度。结果表明:不同材质气管测定CO2浓度的稳定时间为9.20~11.47s,测定H2O气体浓度的稳定时间为9.67~18.93s。利用主效可加互作可乘(Additive main effects and multi-plicative interaction,AMMI)模型对CO2/H2O气体浓度达到稳定的时间进行方差分析和稳定性分析发现,在CO2浓度观测过程中,气管长度的固定效应导致的变异最大,材质次之,材质与长度互作效应较小;各材质中,CO2读数稳定时间最短的为蠕动泵管;在H2O气体浓度观测过程中,存在显著的材质和长度间的互作效应,其中材质的固定效应导致的变异最大,长度次之,PVC管的读数稳定时间最短。不同材质与不同长度的交互作用不同,每种材质对不同长度都有其特殊的适应性。因此,应根据测定指标,选择稳定时间短的材质和长度,以提高农田CO2和H2O气体浓度的测定效率。展开更多
Biochar and biochar-based materials have been studied extensively in multidisciplinary areas because of their outstanding physicochemical properties.In this review article,biochar and biochar-based materials in the re...Biochar and biochar-based materials have been studied extensively in multidisciplinary areas because of their outstanding physicochemical properties.In this review article,biochar and biochar-based materials in the removal of environmental pollutants,hydrogen generation and carbon dioxide capture were summarized and compared.The interaction mechanisms were discussed from the experimental results and characterization analysis.The high porous structures,active surface sites,(co)doping of single metals/nonmetals,and incorporation of metal oxides or other materials improved the high activity of biochar-based materials in their applications.However,there are still some challenges such as:(1)the fact that H_(2) generation with high selectivity or the produced syngas to meet the real application requirement in industrial is the main challenge in H_(2) production;(2)the fact that the selective capture of CO_(2) with high stability,high adsorption capacity and recyclability at low-cost should be considered and focused on;(3)the sorption-(photo)degradation of the organic chemicals;and(4)the fact that the sorption-reduction-extraction/solidification of metals/radionuclides are efficient methods for the elimination of environmental pollutants.In the end,the perspectives,challenges and possible techniques for biochar-based materials’real application in future were described.展开更多
As the greenhouse effect concerns increases,the development of new materials for the efficient capture and separation of CO_(2)gas from gas mixtures has become a matter of urgency.In this study,we performed density fu...As the greenhouse effect concerns increases,the development of new materials for the efficient capture and separation of CO_(2)gas from gas mixtures has become a matter of urgency.In this study,we performed density functional theory(DFT)calculations to investigate the adsorption and separation behavior of CO_(2)/CH_(4)/H_(2)on the surface of two-dimensional(2D)Al_(2)C materials under positive/negative applied electric fields.In the absence of an electric field CO_(2)is weakly physisorbed on the Al_(2)C surface,but with the application of an applied electric field,the adsorption state of CO_(2)gradually changes from physical to chemisorption(adsorption energy changes from-0.29 e V to-3.61 e V),while the negative electric field has little effect on the adsorption of CO_(2).We conclude that the C=O bond in adsorbed CO_(2)can be activated under an external electric field(maximum activation of 15%under an external electric field of 0-0.005 a.u.).Only in the presence of an applied electric field of 0.0033 a.u.and temperatures above525 K/675 K can the adsorption/separation reaction of CO_(2)single adsorption and CO_(2)/CH_(4)/H_(2)mixture be spontaneous.The adsorption/desorption of CO_(2)on Al_(2)C nanosheet in an electric field of 0.003-0.0033 a.u.is all exothermic,which can be easily controlled by switching on/off the electric field without any energy barriers.The capacity of Al_(2)C to capture CO_(2)per unit electric field decreases with increasing CO_(2)concentration,but still has efficient gas separation properties for CO_(2)/CH_(4)/H_(2).Our theoretical results could provide guidance for designing high-capacity and high-selectivity CO_(2)capture materials.展开更多
NH_(3)-SCR is an effective mean of NOxremoval in the non-electric industry, however, the high activation temperature and poor H_(2)O resistance of SCR catalysts posed a barrier to its application. In this work, a seri...NH_(3)-SCR is an effective mean of NOxremoval in the non-electric industry, however, the high activation temperature and poor H_(2)O resistance of SCR catalysts posed a barrier to its application. In this work, a series of three-dimensionally ordered macroporous(3DOM) catalysts were synthesized via a colloidal crystal template(CCT) method, and various characterizations were carried out to explore the physicochemical property of catalysts. The experiment results reveal that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst presents the excellent low-temperature catalytic activity of nearly 100% at 100℃. Furthermore, the enhanced H_(2)O resistance is achieved, certified by the unaffected NO remove at 150℃ in the participation of 15 vol% H_(2)O. The characterizations results exhibit that the improved dispersion of the active component and enhanced redox ability are conducive to the low-temperature catalytic activity. N_(2) adsorption and desorption experiments indicate that catalyst with 3DOM support possesses a larger pore diameter and specific surface area, which may weaken the condensation of H_(2)O in the microporosity of catalysts and improved the H_(2)O resistance of the catalyst. In situ DRIFTS results manifest that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst could not only absorb more NH_(3) and generate more surface-active sites, but inhibit the competitive adsorption between H_(2)O and SCR reactants.展开更多
Recently electrochemical synthesis of H_(2)O_(2)through oxygen reduction reaction(ORR)via 2e^(-)pathway is considered as a green and on-site route.However,it still remains a big challenge for fabricating novel metal-f...Recently electrochemical synthesis of H_(2)O_(2)through oxygen reduction reaction(ORR)via 2e^(-)pathway is considered as a green and on-site route.However,it still remains a big challenge for fabricating novel metal-free catalysts under acidic solutions,since it suffers from high overpotential due to the intrinsically week*OOH adsorption.Herein,a co-doped carbon nanosheet(O/N–C)catalyst toward regulating O and N content was synthesized for improving the selectivity and activity of H_(2)O_(2)electrosynthesis process.The O/N–C exhibits outstanding 2e-ORR performance with low onset potential of 0.4 V(vs.RHE)and a selectivity of 92.4%in 0.1 mol/L HClO_(4)solutions.The in situ electrochemical impedance spectroscopy(EIS)tests reveals that the N incorporation contributes to the fast ORR kinetics.The density functional theory(DFT)calculations demonstrate that the binding strength of*OOH was optimized by the co-doping of oxygen and nitrogen at certain content,and the O/N–C–COOH site exhibits a lower theoretical overpotential for H_(2)O_(2)formation than O–C–COOH site.Furthermore,the promoted kinetics for typical organic dye degradation in simultaneous electron-Fenton process on O/N–C catalyst was demonstrated particularly for broadening its environmental application.展开更多
基金supported by the National Natural Science Foundation of China(Nos.51974225,51874229,51674188,51904224,51904225)the Shaanxi Innovative Talents Cultivate Program-New-star Plan of Science and Technology,China(No.2018KJXX-083)+2 种基金the Natural Science Basic Research Plan of Shaanxi Province of China(Nos.2018JM 5161,2018JQ5183,2019JM-074)the Scientific Research Program funded by the Shaanxi Provincial Education Department,China(No.19JK0543)the Outstanding Youth Science Fund of Xi’an University of Science and Technology,China(No.2018YQ2-01)。
文摘CaCl_(2)·6H_(2)O/expanded vermiculite shape stabilized phase change materials(CEV)was prepared by atmospheric impregnation method.Using gold mine tailings as aggregate of cemented paste backfill(CPB)material,the CPB with CEV added was prepared,and the specific heat capacity,thermal conductivity,and uniaxial compressive strength(UCS)of CPB with different cement-tailing ratios and CEV addition ratios were tested,the influence of the above variables on the thermal and mechanical properties of CPB was analyzed.The results show that the maximum encapsulation capacity of expanded vermiculite for CaCl_(2)·6H_(2)O is about 60%,and the melting and solidification enthalpies of CEV can reach 98.87 J/g and 97.56 J/g,respectively.For the CPB without CEV,the specific heat capacity,thermal conductivity,and UCS decrease with the decrease of cement-tailing ratio.For the CPB with CEV added,with the increase of CEV addition ratio,the specific heat capacity increases significantly,and the sensible heat storage capacity and latent heat storage capacity can be increased by at least 10.74%and 218.97%respectively after adding 12%CEV.However,the addition of CEV leads to the increase of pores,and the thermal conductivity and UCS both decrease with the increase of CEV addition.When cement-tailing ratio is 1:8 and 6%,9%,and 12%of CEV are added,the 28-days UCS of CPB is less than 1 MPa.Considering the heat storage capacity and cost price of backfill,the recommended proportion scheme of CPB material presents cement-tailing ratio of 1:6 and 12%CEV,and the most recommended heat storage/release temperature cycle range of CPB with added CEV is from 20 to 40℃.This work can provide theoretical basis for the utilization of heat storage backfill in green mines.
文摘CO2和H2O气体浓度是农田小气候的2个重要指标,一般采用CO2/H2O分析仪进行测定,为减少人为干扰,需使用气管将待测区域气体传输至分析器,而气管的材质及其长度会影响CO2/H2O测定时读数稳定所需的时间。本研究采用8种常用材质的气管及5种气管长度进行双因素随机区组试验,以筛选CO2/H2O测定所需的最佳气管材质及长度。结果表明:不同材质气管测定CO2浓度的稳定时间为9.20~11.47s,测定H2O气体浓度的稳定时间为9.67~18.93s。利用主效可加互作可乘(Additive main effects and multi-plicative interaction,AMMI)模型对CO2/H2O气体浓度达到稳定的时间进行方差分析和稳定性分析发现,在CO2浓度观测过程中,气管长度的固定效应导致的变异最大,材质次之,材质与长度互作效应较小;各材质中,CO2读数稳定时间最短的为蠕动泵管;在H2O气体浓度观测过程中,存在显著的材质和长度间的互作效应,其中材质的固定效应导致的变异最大,长度次之,PVC管的读数稳定时间最短。不同材质与不同长度的交互作用不同,每种材质对不同长度都有其特殊的适应性。因此,应根据测定指标,选择稳定时间短的材质和长度,以提高农田CO2和H2O气体浓度的测定效率。
基金National Key Research and Development Program of China(2018YFC1900105)National Natural Science Foundation of China(22276054)Beijing Outstanding Young Scientist Program.
文摘Biochar and biochar-based materials have been studied extensively in multidisciplinary areas because of their outstanding physicochemical properties.In this review article,biochar and biochar-based materials in the removal of environmental pollutants,hydrogen generation and carbon dioxide capture were summarized and compared.The interaction mechanisms were discussed from the experimental results and characterization analysis.The high porous structures,active surface sites,(co)doping of single metals/nonmetals,and incorporation of metal oxides or other materials improved the high activity of biochar-based materials in their applications.However,there are still some challenges such as:(1)the fact that H_(2) generation with high selectivity or the produced syngas to meet the real application requirement in industrial is the main challenge in H_(2) production;(2)the fact that the selective capture of CO_(2) with high stability,high adsorption capacity and recyclability at low-cost should be considered and focused on;(3)the sorption-(photo)degradation of the organic chemicals;and(4)the fact that the sorption-reduction-extraction/solidification of metals/radionuclides are efficient methods for the elimination of environmental pollutants.In the end,the perspectives,challenges and possible techniques for biochar-based materials’real application in future were described.
基金funded by the National Natural Science Foundation of China(No.21603109)the Henan Joint Fund of the National Natural Science Foundation of China(No.U1404216)the Scientific Research Program Funded by Shaanxi Provincial Education Department(No.20JK0676)。
文摘As the greenhouse effect concerns increases,the development of new materials for the efficient capture and separation of CO_(2)gas from gas mixtures has become a matter of urgency.In this study,we performed density functional theory(DFT)calculations to investigate the adsorption and separation behavior of CO_(2)/CH_(4)/H_(2)on the surface of two-dimensional(2D)Al_(2)C materials under positive/negative applied electric fields.In the absence of an electric field CO_(2)is weakly physisorbed on the Al_(2)C surface,but with the application of an applied electric field,the adsorption state of CO_(2)gradually changes from physical to chemisorption(adsorption energy changes from-0.29 e V to-3.61 e V),while the negative electric field has little effect on the adsorption of CO_(2).We conclude that the C=O bond in adsorbed CO_(2)can be activated under an external electric field(maximum activation of 15%under an external electric field of 0-0.005 a.u.).Only in the presence of an applied electric field of 0.0033 a.u.and temperatures above525 K/675 K can the adsorption/separation reaction of CO_(2)single adsorption and CO_(2)/CH_(4)/H_(2)mixture be spontaneous.The adsorption/desorption of CO_(2)on Al_(2)C nanosheet in an electric field of 0.003-0.0033 a.u.is all exothermic,which can be easily controlled by switching on/off the electric field without any energy barriers.The capacity of Al_(2)C to capture CO_(2)per unit electric field decreases with increasing CO_(2)concentration,but still has efficient gas separation properties for CO_(2)/CH_(4)/H_(2).Our theoretical results could provide guidance for designing high-capacity and high-selectivity CO_(2)capture materials.
基金Project supported by National Key Research and Development Program of China(2021YFB3500601)。
文摘NH_(3)-SCR is an effective mean of NOxremoval in the non-electric industry, however, the high activation temperature and poor H_(2)O resistance of SCR catalysts posed a barrier to its application. In this work, a series of three-dimensionally ordered macroporous(3DOM) catalysts were synthesized via a colloidal crystal template(CCT) method, and various characterizations were carried out to explore the physicochemical property of catalysts. The experiment results reveal that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst presents the excellent low-temperature catalytic activity of nearly 100% at 100℃. Furthermore, the enhanced H_(2)O resistance is achieved, certified by the unaffected NO remove at 150℃ in the participation of 15 vol% H_(2)O. The characterizations results exhibit that the improved dispersion of the active component and enhanced redox ability are conducive to the low-temperature catalytic activity. N_(2) adsorption and desorption experiments indicate that catalyst with 3DOM support possesses a larger pore diameter and specific surface area, which may weaken the condensation of H_(2)O in the microporosity of catalysts and improved the H_(2)O resistance of the catalyst. In situ DRIFTS results manifest that Ce_(0.2)Mn_(0.2)/3DOM-TiO_(2) catalyst could not only absorb more NH_(3) and generate more surface-active sites, but inhibit the competitive adsorption between H_(2)O and SCR reactants.
基金supported by the National Natural Science Foundation of China(Nos.U22A20432,22278364,22211530045,22178308)the Fundamental Research Funds for the Central Universities(Nos.226-2022-00044,226-2022-00055)+6 种基金the Research Funds of Institute of Zhejiang University-Quzhou(No.IZQ2021KJ2003)National Key Research and Development Program of China(No.2022YFB4002100)the development project of Zhejiang Province's"Jianbing"and"Lingyan"(No.2023C01226)the Startup Foundation for Hundred-Talent Program of Zhejiang Universitythe Science Foundation of Donghai Laboratory(No.DH_(2)022ZY0009)Zhejiang University Global Partnership Fundthe China Postdoctoral Science Foundation(No.2021M702813)。
文摘Recently electrochemical synthesis of H_(2)O_(2)through oxygen reduction reaction(ORR)via 2e^(-)pathway is considered as a green and on-site route.However,it still remains a big challenge for fabricating novel metal-free catalysts under acidic solutions,since it suffers from high overpotential due to the intrinsically week*OOH adsorption.Herein,a co-doped carbon nanosheet(O/N–C)catalyst toward regulating O and N content was synthesized for improving the selectivity and activity of H_(2)O_(2)electrosynthesis process.The O/N–C exhibits outstanding 2e-ORR performance with low onset potential of 0.4 V(vs.RHE)and a selectivity of 92.4%in 0.1 mol/L HClO_(4)solutions.The in situ electrochemical impedance spectroscopy(EIS)tests reveals that the N incorporation contributes to the fast ORR kinetics.The density functional theory(DFT)calculations demonstrate that the binding strength of*OOH was optimized by the co-doping of oxygen and nitrogen at certain content,and the O/N–C–COOH site exhibits a lower theoretical overpotential for H_(2)O_(2)formation than O–C–COOH site.Furthermore,the promoted kinetics for typical organic dye degradation in simultaneous electron-Fenton process on O/N–C catalyst was demonstrated particularly for broadening its environmental application.
