Biomass-H_(2)O gasification is a complex thermochemical reaction,including three processes of volatile removal:homogeneous/heterogeneous reforming,biochar gasification and etching.The rate-determining step is biochar-...Biomass-H_(2)O gasification is a complex thermochemical reaction,including three processes of volatile removal:homogeneous/heterogeneous reforming,biochar gasification and etching.The rate-determining step is biochar-H_(2)O gasification and etching so the DFT is carried out to see the catalytic role of different metal elements(K/Ni)in the zigzag biochar model.The calculation results show that the gasification of biochar-H_(2)O needs to go through four processes:dissociative adsorption of water,hydrogen transfer(hydrogen desorption,hydrogen atom transfer),carbon dissolution and CO desorption.The energy barrier indicated that the most significant step in reducing the activation energy of K is reflected in the hydrogen transfer step,which is reduced from 374.14 kJ/mol to 152.41 kJ/mol;the catalytic effect of Ni is mainly reflected in the carbon dissolution step,which is reduced from 122.34 kJ/mol to 84.8 kJ/mol.The existence of K causes the edge to have a stronger attraction to H and does not destroy theπbonds of biochar molecules.The destruction ofπbonds is mainly due to the role of H free radicals,while the destruction ofπbonds will lead to easier C-C bond rupture.Ni shows a strong attraction to O in OH,which forms strong Ni-O chemical bonds.Ni can also destroy the aromatic structure directly,making the gasification easier to happen.This study explored the catalytic mechanism of K/Ni on the biochar-H_(2)O gasification at the molecular level and looked forward to the potential synergy of K/Ni,laying a foundation for experimental research and catalyst design.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
基金Sponsored by the National Natural Science Foundation of China(Grant No.52276180)the Natural Science Foundation of Heilongjiang Province(Grant No.YQ2022E026).
文摘Biomass-H_(2)O gasification is a complex thermochemical reaction,including three processes of volatile removal:homogeneous/heterogeneous reforming,biochar gasification and etching.The rate-determining step is biochar-H_(2)O gasification and etching so the DFT is carried out to see the catalytic role of different metal elements(K/Ni)in the zigzag biochar model.The calculation results show that the gasification of biochar-H_(2)O needs to go through four processes:dissociative adsorption of water,hydrogen transfer(hydrogen desorption,hydrogen atom transfer),carbon dissolution and CO desorption.The energy barrier indicated that the most significant step in reducing the activation energy of K is reflected in the hydrogen transfer step,which is reduced from 374.14 kJ/mol to 152.41 kJ/mol;the catalytic effect of Ni is mainly reflected in the carbon dissolution step,which is reduced from 122.34 kJ/mol to 84.8 kJ/mol.The existence of K causes the edge to have a stronger attraction to H and does not destroy theπbonds of biochar molecules.The destruction ofπbonds is mainly due to the role of H free radicals,while the destruction ofπbonds will lead to easier C-C bond rupture.Ni shows a strong attraction to O in OH,which forms strong Ni-O chemical bonds.Ni can also destroy the aromatic structure directly,making the gasification easier to happen.This study explored the catalytic mechanism of K/Ni on the biochar-H_(2)O gasification at the molecular level and looked forward to the potential synergy of K/Ni,laying a foundation for experimental research and catalyst design.
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。
