The combined effects of straw incorporation(SI)and polymer-coated urea(PCU)application on soil ammonia(NH_(3))and nitrous oxide(N_(2)O)emissions from agricultural fields have not been comprehensively evaluated in Nort...The combined effects of straw incorporation(SI)and polymer-coated urea(PCU)application on soil ammonia(NH_(3))and nitrous oxide(N_(2)O)emissions from agricultural fields have not been comprehensively evaluated in Northwest China.We conducted a two-year field experiment to assess the effects of combining SI with either uncoated urea(U)or PCU on soil NH_(3)emissions,N_(2)O emissions,winter wheat yields,yield-scaled NH_(3)(/NH_(3)),and yield-scaled N_(2)O(/N_(2)O).Five treatments were investigated,no nitrogen(N)fertilizer(N_(0)),U application at 150 kg N ha-1 with and without SI(SI+U and S_(0)+U),and PCU application at 150 kg N ha^(-1) with and without SI(SI+PCU and S_(0)+PCU).The results showed that the NH_(3);emissions increased by 20.98-34.35%following Sl compared to straw removal,mainly due to increases in soil ammonium(NH_(4)^(+)-N)content and water-flled pore space(WFPS).SI resulted in higher N_(2)O emissions than under the So scenario by 13.31-49.23%due to increases in soil inorganic N(SIN)contents,WFPS,and soil microbial biomass.In contrast,the PCU application reduced the SIN contents compared to the U application,reducing the NH_(3)and N_(2)O emissions by 45.99-58.07 and 18.08-53.04%,respectively.Moreover,no significant positive effects of the SI or PCU applications on the winter wheat yield were observed.The lowest /NH_(3) and /N_(2)O values were observed under the S_(0)+PCU and SI+PCU treatments.Our results suggest that single PCU applications and their combination with straw are the optimal agricultural strategies for mitigating gaseous N emissions and maintaining optimal winter wheat yields in Northwest China.展开更多
Cobalt-rich perovskite oxides play a paramount role in catalyzing oxygen evolution reaction(OER)on account of their acceptable intrinsic activity but are still challenging due to the high costs and undesired stability...Cobalt-rich perovskite oxides play a paramount role in catalyzing oxygen evolution reaction(OER)on account of their acceptable intrinsic activity but are still challenging due to the high costs and undesired stability.In response to the defects,herein,the Mg-incorporated perovskite cobaltite SrCo_(0.6)Fe_(0.3M)g_(0.1)O_(3-δ)(SCFM-0.1)is proposed as a novel earth-abundant and durable OER electrocatalyst.A well-consolidated cubic-symmetry structure and more active oxygen intermediates are enabled upon Mg substitution.Hence,the optimized SCFM-0.1 perovskite oxide achieves prominent OER electrocatalytic performance,that is,a low overpotential of only 320 mV at 10 mA cm^(-2),a small Tafel slope of 65 mV dec^(-1),as well as an outstanding durability within 20 h,substantially outperforming that of the pristine SrCo_(0.7)Fe_(0.3)O_(3-δ)and benchmark Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3-δ)and IrO_(2) catalysts.The strong pHdependent behavior associated with lattice oxygen activation mechanism for SCFM-0.1 catalyst is also confirmed.This work paves a unique avenue to develop cost-effective and robust perovskite cobaltites for efficient OER electrocatalysis.展开更多
秸秆还田与氮肥施用是农田生态系统中碳氮元素的两大主要补给途径,其在调控稻田甲烷(CH_(4))和氧化亚氮(N_(2)O)排放以及水稻产量方面具有重要作用。以往的研究主要关注秸秆还田或氮肥施用单因素对稻田温室气体排放的影响,而双因素互作...秸秆还田与氮肥施用是农田生态系统中碳氮元素的两大主要补给途径,其在调控稻田甲烷(CH_(4))和氧化亚氮(N_(2)O)排放以及水稻产量方面具有重要作用。以往的研究主要关注秸秆还田或氮肥施用单因素对稻田温室气体排放的影响,而双因素互作对甲烷和氧化亚氮排放的影响尚未明确。同时,在秸秆还田条件下如何进行合理的氮肥施用鲜有深入研究。本研究基于3个氮肥处理(0、180、360 kg N/hm^(2))和3个秸秆还田处理(0、2.25、3.75 t/hm^(2))进行多年水稻田间定位试验,研究结果表明:CH_(4)季节累积排放随秸秆还田量增加而增加,与施氮量无显著正相关关系;N_(2)O季节累积排放随施氮量增加而增加,与秸秆还田量无显著正相关关系;秸秆还田对于产量的影响具有不确定性,两年均在秸秆不还田+不施氮处理(S0N0)出现最低产量,2021与2022年最低产量分别为5740.64和4903.75 kg/hm^(2)。2021与2022年最高产量分别在秸秆不还田+高氮(S0N_(2))和高量秸秆还田+高氮(S2N_(2))出现,分别为10938.48和10384.83 kg/hm^(2)。同时,本研究发现在低量秸秆还田条件下,在碳足迹(CF, Carbon Footprint)方面,施氮量为251 kg N/hm^(2)时碳足迹达到最低点,为1.01 kg C/kg;而在生态经济净收益(NEEB, Net Ecosystem Economic Benefits)方面,施氮量为294 kg N/hm^(2)时生态经济净收益达到最高点,为11778.15元/hm^(2)。为协同生态经济净收益与碳排放,在低量秸秆还田(S1)下,配合251—294 kg N/hm^(2)的施氮量为最优施肥方案。研究结果为指导稻田温室气体减排、实现稻田碳中和以及农田管理提供了理论支撑,为实现水稻的高产稳产与低碳生产科学依据。展开更多
Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy ...Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.展开更多
基金This work was supported by the National Key R&D Program of China(2021YFD1900700)the National Natural Science Foundation of China(52179046).
文摘The combined effects of straw incorporation(SI)and polymer-coated urea(PCU)application on soil ammonia(NH_(3))and nitrous oxide(N_(2)O)emissions from agricultural fields have not been comprehensively evaluated in Northwest China.We conducted a two-year field experiment to assess the effects of combining SI with either uncoated urea(U)or PCU on soil NH_(3)emissions,N_(2)O emissions,winter wheat yields,yield-scaled NH_(3)(/NH_(3)),and yield-scaled N_(2)O(/N_(2)O).Five treatments were investigated,no nitrogen(N)fertilizer(N_(0)),U application at 150 kg N ha-1 with and without SI(SI+U and S_(0)+U),and PCU application at 150 kg N ha^(-1) with and without SI(SI+PCU and S_(0)+PCU).The results showed that the NH_(3);emissions increased by 20.98-34.35%following Sl compared to straw removal,mainly due to increases in soil ammonium(NH_(4)^(+)-N)content and water-flled pore space(WFPS).SI resulted in higher N_(2)O emissions than under the So scenario by 13.31-49.23%due to increases in soil inorganic N(SIN)contents,WFPS,and soil microbial biomass.In contrast,the PCU application reduced the SIN contents compared to the U application,reducing the NH_(3)and N_(2)O emissions by 45.99-58.07 and 18.08-53.04%,respectively.Moreover,no significant positive effects of the SI or PCU applications on the winter wheat yield were observed.The lowest /NH_(3) and /N_(2)O values were observed under the S_(0)+PCU and SI+PCU treatments.Our results suggest that single PCU applications and their combination with straw are the optimal agricultural strategies for mitigating gaseous N emissions and maintaining optimal winter wheat yields in Northwest China.
基金supported by the National Natural Science Foundation of China(No.22108043)Natural Science Foundation of Guangdong Province,China(No.2023A1515012711).
文摘Cobalt-rich perovskite oxides play a paramount role in catalyzing oxygen evolution reaction(OER)on account of their acceptable intrinsic activity but are still challenging due to the high costs and undesired stability.In response to the defects,herein,the Mg-incorporated perovskite cobaltite SrCo_(0.6)Fe_(0.3M)g_(0.1)O_(3-δ)(SCFM-0.1)is proposed as a novel earth-abundant and durable OER electrocatalyst.A well-consolidated cubic-symmetry structure and more active oxygen intermediates are enabled upon Mg substitution.Hence,the optimized SCFM-0.1 perovskite oxide achieves prominent OER electrocatalytic performance,that is,a low overpotential of only 320 mV at 10 mA cm^(-2),a small Tafel slope of 65 mV dec^(-1),as well as an outstanding durability within 20 h,substantially outperforming that of the pristine SrCo_(0.7)Fe_(0.3)O_(3-δ)and benchmark Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3-δ)and IrO_(2) catalysts.The strong pHdependent behavior associated with lattice oxygen activation mechanism for SCFM-0.1 catalyst is also confirmed.This work paves a unique avenue to develop cost-effective and robust perovskite cobaltites for efficient OER electrocatalysis.
文摘秸秆还田与氮肥施用是农田生态系统中碳氮元素的两大主要补给途径,其在调控稻田甲烷(CH_(4))和氧化亚氮(N_(2)O)排放以及水稻产量方面具有重要作用。以往的研究主要关注秸秆还田或氮肥施用单因素对稻田温室气体排放的影响,而双因素互作对甲烷和氧化亚氮排放的影响尚未明确。同时,在秸秆还田条件下如何进行合理的氮肥施用鲜有深入研究。本研究基于3个氮肥处理(0、180、360 kg N/hm^(2))和3个秸秆还田处理(0、2.25、3.75 t/hm^(2))进行多年水稻田间定位试验,研究结果表明:CH_(4)季节累积排放随秸秆还田量增加而增加,与施氮量无显著正相关关系;N_(2)O季节累积排放随施氮量增加而增加,与秸秆还田量无显著正相关关系;秸秆还田对于产量的影响具有不确定性,两年均在秸秆不还田+不施氮处理(S0N0)出现最低产量,2021与2022年最低产量分别为5740.64和4903.75 kg/hm^(2)。2021与2022年最高产量分别在秸秆不还田+高氮(S0N_(2))和高量秸秆还田+高氮(S2N_(2))出现,分别为10938.48和10384.83 kg/hm^(2)。同时,本研究发现在低量秸秆还田条件下,在碳足迹(CF, Carbon Footprint)方面,施氮量为251 kg N/hm^(2)时碳足迹达到最低点,为1.01 kg C/kg;而在生态经济净收益(NEEB, Net Ecosystem Economic Benefits)方面,施氮量为294 kg N/hm^(2)时生态经济净收益达到最高点,为11778.15元/hm^(2)。为协同生态经济净收益与碳排放,在低量秸秆还田(S1)下,配合251—294 kg N/hm^(2)的施氮量为最优施肥方案。研究结果为指导稻田温室气体减排、实现稻田碳中和以及农田管理提供了理论支撑,为实现水稻的高产稳产与低碳生产科学依据。
基金supported by the National Natural Science Foundation of China(52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD18126001,GUIKE AD20297039)。
文摘Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.