The laminar combustion characteristics of CH_(4)/air premixed flames with CO_(2) addition are systemically studied.Experimental measurements and numerical simulations of the laminar burning velocity(LBV)are performed ...The laminar combustion characteristics of CH_(4)/air premixed flames with CO_(2) addition are systemically studied.Experimental measurements and numerical simulations of the laminar burning velocity(LBV)are performed in CH_(4)/CO_(2)/Air flames with various CO_(2) doping ratio under equivalence ratios of 1.0–1.4.GRI 3.0 mech and Aramco mech are employed for predicting LBV,adiabatic flame temperature(AFT),important intermediate radicals(CH_(3),H,OH,O)and NO_(x) emissions(NO,NO_(2),N2O),as well as the sensitivity analysis is also conducted.The detail analysis of experiment and simulation reveals that as the CO_(2) addition increases from 0%to 40%,the LBVs and AFTs decrease monotonously.Under the same CO_(2) doping ratio,the LBVs and AFTs increase first and then decrease with the increase of equivalence ratio,and the maximum of LBV is reached at equivalence ratio of 1.05.The mole fraction tendency of important intermediates and NO_(x) with equivalence ratio and CO_(2) doping ratio are similar to the LBVs and AFTs.Reaction H+O_(2)⇔O+OH is found to be responsible for the promotion of the generation of important intermediates and NO_(x) under the equivalence ratios and CO_(2) addition through sensitivity analysis.The sensitivity coefficients of elementary reactions that the increasing of CO_(2) doping ratio promotes or inhibits formation of intermediate radicals and NO_(x) decreases.展开更多
Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic a...Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic activity and selectivity.The mobility and accessibility of active sites in Cubased catalysts significantly hinder the development of efficient Cu-based catalysts for CO_(2)electrochemical reduction reaction(CO_(2)RR).Herein,a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride(g-C_(3)N_(4))as the active sites for CO_(2)-to-CH_(4)conversion in CO_(2)RR.By regulating the coordination and density of Cu sites in g-C_(3)N_(4),an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH_(4)Faraday efficiency of 49.04%and produces the products with a high CH_(4)/C_(2)H_(4)ratio over 9.This work provides the first experimental study on g-C_(3)N_(4)-supported single Cu atom catalyst for efficient CH_(4)production from CO_(2)RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO_(2)RR by engineering Cu active sites in 2D materials with porous crystal structures.展开更多
基金The authors would like to thank the National Natural Science Foundation of China(52176095)Anhui Provincial Natural Science Foundation(2008085J25)the Project of support program for outstanding young people in Colleges and Universities(gxyqZD201830)for their financial support of this study.
文摘The laminar combustion characteristics of CH_(4)/air premixed flames with CO_(2) addition are systemically studied.Experimental measurements and numerical simulations of the laminar burning velocity(LBV)are performed in CH_(4)/CO_(2)/Air flames with various CO_(2) doping ratio under equivalence ratios of 1.0–1.4.GRI 3.0 mech and Aramco mech are employed for predicting LBV,adiabatic flame temperature(AFT),important intermediate radicals(CH_(3),H,OH,O)and NO_(x) emissions(NO,NO_(2),N2O),as well as the sensitivity analysis is also conducted.The detail analysis of experiment and simulation reveals that as the CO_(2) addition increases from 0%to 40%,the LBVs and AFTs decrease monotonously.Under the same CO_(2) doping ratio,the LBVs and AFTs increase first and then decrease with the increase of equivalence ratio,and the maximum of LBV is reached at equivalence ratio of 1.05.The mole fraction tendency of important intermediates and NO_(x) with equivalence ratio and CO_(2) doping ratio are similar to the LBVs and AFTs.Reaction H+O_(2)⇔O+OH is found to be responsible for the promotion of the generation of important intermediates and NO_(x) under the equivalence ratios and CO_(2) addition through sensitivity analysis.The sensitivity coefficients of elementary reactions that the increasing of CO_(2) doping ratio promotes or inhibits formation of intermediate radicals and NO_(x) decreases.
基金This work was supported by the Fundamental Research Funds for the Central Universities(2232021A-02 and 2232023Y-01)the National Natural Science Foundation of China(Nos.52122312,22209024 and 22202183).
文摘Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic activity and selectivity.The mobility and accessibility of active sites in Cubased catalysts significantly hinder the development of efficient Cu-based catalysts for CO_(2)electrochemical reduction reaction(CO_(2)RR).Herein,a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride(g-C_(3)N_(4))as the active sites for CO_(2)-to-CH_(4)conversion in CO_(2)RR.By regulating the coordination and density of Cu sites in g-C_(3)N_(4),an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH_(4)Faraday efficiency of 49.04%and produces the products with a high CH_(4)/C_(2)H_(4)ratio over 9.This work provides the first experimental study on g-C_(3)N_(4)-supported single Cu atom catalyst for efficient CH_(4)production from CO_(2)RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO_(2)RR by engineering Cu active sites in 2D materials with porous crystal structures.
文摘选择造林树种大叶相思(Acacia auriculiformis)和樟树(Cinnamomum camphora)为对象,采用开顶生长箱(open-top chamber,OTC)构建实验林,探讨镉(Cd)胁迫及其与大气CO_(2)浓度升高、氮(N)添加的复合作用对2种树木叶片N、P养分利用策略和Cd积累特征的影响。试验设5个处理:对照(CK)、加Cd[10 kg Cd/(hm^(2)·a)](Cd)、加Cd与加CO_(2)(700μmol/mol)(CdC)、加Cd与加N[100 kg N/(hm^(2)·a)](CdN)、加Cd加CO_(2)加N(CdCN)。处理约2.5 a后,测定两树种的成熟叶和衰老叶中N、磷(P)和Cd含量。结果表明,不同处理对两树种叶片P含量及P回收率均无显著影响,但显著影响叶片N含量及N回收率;CdN处理下两树种叶片N含量升高;Cd和CdN处理下樟树叶N回收率显著降低。Cd、CdC、CdN和CdCN处理下两树种叶片Cd积累浓度及樟树成熟叶中的Cd/N和Cd/P升高。大叶相思叶片N、P回收率显著高于樟树,Cd积累浓度显著低于樟树。速生豆科固氮树种大叶相思比普通非固氮树种樟树具有更好的N、P养分利用策略和抵御叶片积累Cd的能力,表明大叶相思可以作为Cd污染林地土壤生态修复的适宜树种。
