Due to increasing global demand for crop production and energy use, more and more reactive nitrogen(Nr) has been generated and emitted to the environment. As a result, global atmospheric nitrogen(N) deposition has...Due to increasing global demand for crop production and energy use, more and more reactive nitrogen(Nr) has been generated and emitted to the environment. As a result, global atmospheric nitrogen(N) deposition has tripled since the industrial revolution and the ecological environment and human health have been harmed. In this study, we measured dry and wet/bulk N deposition from July 2013 to December 2015 in a semi-arid grassland of Duolun County, Inner Mongolia, China. The samples of dry and wet/bulk N deposition were collected monthly with a DELTA(DEnuder for Long Term Atmospheric sampling) system and with Gradko passive samplers and a precipitation gauge. The measured results show that the annual mean concentrations of NH_3, NO_2, HNO_3, particulate NH_4~+(pNH_4~+) and particulate NO_3^-(pNO_3^-) in atmosphere were 2.33, 1.90, 0.18, 1.42 and 0.42 μg N/m3, respectively, and that the annual mean volume-weighted concentrations of NH_4~+-N and NO_3^--N in precipitation were 2.71 and 1.99 mg N/L, respectively. The concentrations of Nr components(including NH_3, NO_2, HNO_3, p NH_4~+, pNO_3^-, NH_4~+-N and NO_3^--N) exhibited different seasonal variations. Specifically, NO_2 and HNO_3 exhibited higher concentrations in autumn than in summer, while the other Nr components(NH_3, pNH_4~+, pNO_3^-, NH_4~+-N and NO_3^--N) showed the highest values in summer. Based on measured concentrations of Nr components and their deposition velocities estimated using the GEOS-Chem global atmospheric chemical transport model, the calculated annual mean dry deposition fluxes were 3.17, 1.13, 0.63, 0.91 and 0.36 kg N/(hm^2·a) for NH_3, NO_2, HNO_3, p NH_4~+ and pNO_3^-, respectively, and the calculated annual mean wet/bulk deposition fluxes were 5.37 and 3.15 kg N/(hm^2·a) for NH_4~+-N and NO_3^--N, respectively. The estimated annual N deposition(including dry N deposition and wet/bulk N deposition) reached 14.7 kg N/(hm^2·a) in grassland of Duolun County, approaching to the upper limit of the N critical load(10–15 kg N/(hm^2·a)). Dry and wet/bulk deposition fluxes of all Nr components(with an exception of HNO_3) showed similar seasonal variations with the maximum deposition flux in summer and the minimum in winter. Reduced Nr components(e.g., gaseous NH_3 and p NH_4~+ in atmosphere and NH_4~+-N in precipitation) dominated the total N deposition at the sampling site(accounted for 64% of the total N deposition), suggesting that the deposited atmospheric Nr mainly originated from agricultural activities. Considering the projected future increases in crop and livestock production in Inner Mongolia, the ecological and human risks to the negative effects of increased N deposition could be increased if no mitigation measures are taken.展开更多
Lithium (Li) metal is considered as one of the most promising anode materials to build next-generation high-energy–density batteries. Nonetheless, dendritic Li deposition has dramatically hindered the practical appli...Lithium (Li) metal is considered as one of the most promising anode materials to build next-generation high-energy–density batteries. Nonetheless, dendritic Li deposition has dramatically hindered the practical applications of Li metal batteries (LMBs). Uniformizing Li deposition is a prerequisite to achieve safe and practical LMBs. Herein, an underpotential deposition (UPD) process is first proposed to alter the kinetic and uniformity of Li deposition morphology. Based on the strong interaction between the Li adatoms and manganese (Mn) based substrate, a competition between the UPD and bulk Li deposition is observed, on which the predominance of the UPD scenario tends to uniformize Li nucleation and deposition by the surface coverage of Li monolayers at potentials that are more positive than the Nernst potential of Li metal. Inspired by this process, an advanced hybrid Mn-graphene oxide structure is developed for Li protection, not only enabling dendrite-free Li anodes for high-capacity and -current density cycling, but also improving the interfacial kinetic of Li metal anodes at subzero temperatures, showing potential applicability in low temperature conditions.展开更多
基金financially supported by the National Key R&D Program of China (2017YFC0210101, 2014CB954202)the National Natural Science Foundation of China (41425007)
文摘Due to increasing global demand for crop production and energy use, more and more reactive nitrogen(Nr) has been generated and emitted to the environment. As a result, global atmospheric nitrogen(N) deposition has tripled since the industrial revolution and the ecological environment and human health have been harmed. In this study, we measured dry and wet/bulk N deposition from July 2013 to December 2015 in a semi-arid grassland of Duolun County, Inner Mongolia, China. The samples of dry and wet/bulk N deposition were collected monthly with a DELTA(DEnuder for Long Term Atmospheric sampling) system and with Gradko passive samplers and a precipitation gauge. The measured results show that the annual mean concentrations of NH_3, NO_2, HNO_3, particulate NH_4~+(pNH_4~+) and particulate NO_3^-(pNO_3^-) in atmosphere were 2.33, 1.90, 0.18, 1.42 and 0.42 μg N/m3, respectively, and that the annual mean volume-weighted concentrations of NH_4~+-N and NO_3^--N in precipitation were 2.71 and 1.99 mg N/L, respectively. The concentrations of Nr components(including NH_3, NO_2, HNO_3, p NH_4~+, pNO_3^-, NH_4~+-N and NO_3^--N) exhibited different seasonal variations. Specifically, NO_2 and HNO_3 exhibited higher concentrations in autumn than in summer, while the other Nr components(NH_3, pNH_4~+, pNO_3^-, NH_4~+-N and NO_3^--N) showed the highest values in summer. Based on measured concentrations of Nr components and their deposition velocities estimated using the GEOS-Chem global atmospheric chemical transport model, the calculated annual mean dry deposition fluxes were 3.17, 1.13, 0.63, 0.91 and 0.36 kg N/(hm^2·a) for NH_3, NO_2, HNO_3, p NH_4~+ and pNO_3^-, respectively, and the calculated annual mean wet/bulk deposition fluxes were 5.37 and 3.15 kg N/(hm^2·a) for NH_4~+-N and NO_3^--N, respectively. The estimated annual N deposition(including dry N deposition and wet/bulk N deposition) reached 14.7 kg N/(hm^2·a) in grassland of Duolun County, approaching to the upper limit of the N critical load(10–15 kg N/(hm^2·a)). Dry and wet/bulk deposition fluxes of all Nr components(with an exception of HNO_3) showed similar seasonal variations with the maximum deposition flux in summer and the minimum in winter. Reduced Nr components(e.g., gaseous NH_3 and p NH_4~+ in atmosphere and NH_4~+-N in precipitation) dominated the total N deposition at the sampling site(accounted for 64% of the total N deposition), suggesting that the deposited atmospheric Nr mainly originated from agricultural activities. Considering the projected future increases in crop and livestock production in Inner Mongolia, the ecological and human risks to the negative effects of increased N deposition could be increased if no mitigation measures are taken.
基金This work was supported by the 21C Innovation Laboratory,Contemporary Amperex Technology Ltd by project No.21C-OP-202004the Ningbo 2025 Project(Grant No.2018B10061,2018B10087 and 2019B10044)+1 种基金the National Key R&D Program of China(Grant No.2018YFB0905400)the National Natural Science Foundation of China(Grant No.21805297).
文摘Lithium (Li) metal is considered as one of the most promising anode materials to build next-generation high-energy–density batteries. Nonetheless, dendritic Li deposition has dramatically hindered the practical applications of Li metal batteries (LMBs). Uniformizing Li deposition is a prerequisite to achieve safe and practical LMBs. Herein, an underpotential deposition (UPD) process is first proposed to alter the kinetic and uniformity of Li deposition morphology. Based on the strong interaction between the Li adatoms and manganese (Mn) based substrate, a competition between the UPD and bulk Li deposition is observed, on which the predominance of the UPD scenario tends to uniformize Li nucleation and deposition by the surface coverage of Li monolayers at potentials that are more positive than the Nernst potential of Li metal. Inspired by this process, an advanced hybrid Mn-graphene oxide structure is developed for Li protection, not only enabling dendrite-free Li anodes for high-capacity and -current density cycling, but also improving the interfacial kinetic of Li metal anodes at subzero temperatures, showing potential applicability in low temperature conditions.