Ab initio calculations based on density functional theory have been used to study thedecompsition of N_2O on MgO. The reaction is predicted to occur on O_3c and O_(4c) atoms, but not onO_(5c) atoms, with an activation...Ab initio calculations based on density functional theory have been used to study thedecompsition of N_2O on MgO. The reaction is predicted to occur on O_3c and O_(4c) atoms, but not onO_(5c) atoms, with an activation barrier of 25-27 kcal/mol, in agreement with the experimental valueof 35 kcal/mol. Natural bond orbital analysis shows that the reaction leaves O ad-atoms on thosesurface O anions to form a peroxide-like 'O^2_(2-)' species. The )O-O bond stretching frequency ispredicted to be in the range from 820 cm(-1) to 825 cm(-1).展开更多
Three groups of cobalt mixed oxide catalysts（Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co）were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on...Three groups of cobalt mixed oxide catalysts（Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co）were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on cobalt mixed catalysts for nitrous oxide（N2O）decomposing to N2 and O2were investigated. The experimental results revealed that the catalytic activity for N2 O decomposition was promoted as Co2＋was replaced partially by Zn2＋/Mg2＋, moreover, the characterization analysis by XRD and XPS showed that Zn2＋/Mg2＋replaced Co2＋successfully into the spinel structure of Co3O4 and promoted significantly the catalytic activity. Especially, the addition of CeO2 and K2O/Na2O decreased the binding energy and resulted in an increase in the density of the electron cloud around Co and an improvement of the catalytic activity. Of the investigated cobalt mixed catalysts, the best catalytic activity was shown by 2% K-Zn0.5-Ce0.05-Co catalyst.展开更多
优化氮肥施用和秸秆还田技术为途径的农业管理措施被认为是提升农业可持续性的有效手段,然而当前关于氮肥和秸秆还田对小麦产量和N_(2)O排放影响的研究仍十分有限。为此,本研究基于2000—2022年发表的关于长江中下游流域氮肥和秸秆投入...优化氮肥施用和秸秆还田技术为途径的农业管理措施被认为是提升农业可持续性的有效手段,然而当前关于氮肥和秸秆还田对小麦产量和N_(2)O排放影响的研究仍十分有限。为此,本研究基于2000—2022年发表的关于长江中下游流域氮肥和秸秆投入下小麦产量和N_(2)O排放变化的文献,运用随机森林建模,定量分析氮肥和秸秆还田对小麦产量和N_(2)O排放的影响,并结合情景设置进行了特定地点的小麦产量和N_(2)O排放模拟,同时评估了碳排放强度(CEE)和净生态系统经济效益(NEEB)。结果表明,建立的区域尺度小麦产量与N_(2)O排放对氮秸互作响应的随机森林模型,验证结果R^(2)分别为0.66和0.65,RMSE分别为0.70和1.11。结果表明施氮量和土壤有机质是影响小麦产量和N_(2)O排放的重要因素。综合来看,达到最大产量所需的氮肥量为208~212 kg hm^(-2),达到最小CEE所需的氮肥量为113~130 kg hm^(-2),达到最高的NEEB所需的氮肥量为202~205 kg hm^(-2),其中在6.75 t hm^(-2)的秸秆投入下施用202 kg hm^(-2)的氮肥可以获得最高的生态收益1.37万元。优化氮肥和秸秆投入具备减少作物碳排放强度并获得最大净生态环境效益的潜力。展开更多
文摘Ab initio calculations based on density functional theory have been used to study thedecompsition of N_2O on MgO. The reaction is predicted to occur on O_3c and O_(4c) atoms, but not onO_(5c) atoms, with an activation barrier of 25-27 kcal/mol, in agreement with the experimental valueof 35 kcal/mol. Natural bond orbital analysis shows that the reaction leaves O ad-atoms on thosesurface O anions to form a peroxide-like 'O^2_(2-)' species. The )O-O bond stretching frequency ispredicted to be in the range from 820 cm(-1) to 825 cm(-1).
基金supported by the Hi-Tech Research and Development Program (863) of China (No. 2012AA062501)the Natural Science Foundation of Hubei Province (No. 2009CDB246)the Postgraduates Innovation Foundation of Huazhong University of Science and Technology of China (No. HF-08-11-2011-261)
文摘Three groups of cobalt mixed oxide catalysts（Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co）were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on cobalt mixed catalysts for nitrous oxide（N2O）decomposing to N2 and O2were investigated. The experimental results revealed that the catalytic activity for N2 O decomposition was promoted as Co2＋was replaced partially by Zn2＋/Mg2＋, moreover, the characterization analysis by XRD and XPS showed that Zn2＋/Mg2＋replaced Co2＋successfully into the spinel structure of Co3O4 and promoted significantly the catalytic activity. Especially, the addition of CeO2 and K2O/Na2O decreased the binding energy and resulted in an increase in the density of the electron cloud around Co and an improvement of the catalytic activity. Of the investigated cobalt mixed catalysts, the best catalytic activity was shown by 2% K-Zn0.5-Ce0.05-Co catalyst.
文摘优化氮肥施用和秸秆还田技术为途径的农业管理措施被认为是提升农业可持续性的有效手段,然而当前关于氮肥和秸秆还田对小麦产量和N_(2)O排放影响的研究仍十分有限。为此,本研究基于2000—2022年发表的关于长江中下游流域氮肥和秸秆投入下小麦产量和N_(2)O排放变化的文献,运用随机森林建模,定量分析氮肥和秸秆还田对小麦产量和N_(2)O排放的影响,并结合情景设置进行了特定地点的小麦产量和N_(2)O排放模拟,同时评估了碳排放强度(CEE)和净生态系统经济效益(NEEB)。结果表明,建立的区域尺度小麦产量与N_(2)O排放对氮秸互作响应的随机森林模型,验证结果R^(2)分别为0.66和0.65,RMSE分别为0.70和1.11。结果表明施氮量和土壤有机质是影响小麦产量和N_(2)O排放的重要因素。综合来看,达到最大产量所需的氮肥量为208~212 kg hm^(-2),达到最小CEE所需的氮肥量为113~130 kg hm^(-2),达到最高的NEEB所需的氮肥量为202~205 kg hm^(-2),其中在6.75 t hm^(-2)的秸秆投入下施用202 kg hm^(-2)的氮肥可以获得最高的生态收益1.37万元。优化氮肥和秸秆投入具备减少作物碳排放强度并获得最大净生态环境效益的潜力。
