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Cationic ordering transition in oxygen-redox layered oxide cathodes
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作者 Xinyan Li Ang Gao +10 位作者 Qinghua Zhang Hao Yu Pengxiang Ji Dongdong Xiao Xuefeng Wang Dong Su Xiaohui Rong Xiqian Yu Hong Li Yong-Sheng Hu Lin Gu 《Carbon Energy》 SCIE EI CAS CSCD 2024年第1期197-206,共10页
Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na... Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na-ion cathodes.Here,we reveal the correlation between cationic ordering transition and OR degradation in ribbon-ordered P3-Na_(0.6)Li_(0.2)Mn_(0.8)O_(2) via in situ structural analysis.Comparing two different voltage windows,the OR capacity can be improved approximately twofold when suppressing the in-plane cationic ordering transition.We find that the intralayer cationic migration is promoted by electrochemical reduction from Mn^(4+)to Jahn–Teller Mn^(3+)and the concomitant NaO_(6) stacking transformation from triangular prisms to octahedra,resulting in the loss of ribbon ordering and electrochemical decay.First-principles calculations reveal that Mn^(4+)/Mn^(3+)charge ordering and alignment of the degenerate eg orbital induce lattice-level collective Jahn–Teller distortion,which favors intralayer Mn-ion migration and thereby accelerates OR degradation.These findings unravel the relationship between in-plane cationic ordering and OR reversibility and highlight the importance of superstructure protection for the rational design of reversible OR-active layered oxide cathodes. 展开更多
关键词 cationic ordering layered oxide cathodes oxygen redox sodium-ion batteries
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Designing ultrastable P2/O3-type layered oxides for sodium ion batteries by regulating Na distribution and oxygen redox chemistry
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作者 Jieyou Huang Weiliang Li +3 位作者 Debin Ye Lin Xu Wenwei Wu Xuehang Wu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第7期466-476,共11页
P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phas... P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs. 展开更多
关键词 Sodium-ion batteries P2/O3-type layered oxides Na distribution oxygen redox chemistry Hydrostability
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Effects of tropical forest conversion into oil palm plantations on nitrous oxide emissions:A meta-analysis 被引量:1
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作者 Taiki Mori 《Journal of Forestry Research》 SCIE CAS CSCD 2023年第3期865-869,共5页
Oil palm plantations have dramatically expanded in tropical Asia over the past decades.Although their establishment has been projected to increase nitrous oxide(N_(2)O)emissions,earlier reports have shown inconsistent... Oil palm plantations have dramatically expanded in tropical Asia over the past decades.Although their establishment has been projected to increase nitrous oxide(N_(2)O)emissions,earlier reports have shown inconsistent results.This study analyzed these previously published data to compare N_(2)O emissions in oil palm plantations to reference forests.A linear mixed-eff ects model was used to examine the signifi cance of the eff ect of establishing oil palm plantations on N_(2)O emissions,rather than to calculate mean eff ect sizes because of limitations in the data structure.The results indicated that N_(2)O emissions were signifi cantly greater from oil palm plantations than from reference forests,as expected.This is the fi rst study to report the eff ect of oil palm plantations on N_(2)O emissions by synthesizing previously published data.To quantify the size of this eff ect,additional studies with frequent and long-term monitoring data are needed. 展开更多
关键词 META-ANALYSIS Nitrogen fertilization nitrous oxide Oil palm plantation Tropical forest
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Simultaneous generation of electricity, ethylene and decomposition of nitrous oxide via protonic ceramic fuel cell membrane reactor
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作者 Song Lei Ao Wang +3 位作者 Guowei Weng Ying Wu Jian Xue Haihui Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第2期359-368,I0010,共11页
Ethylene,one of the most widely produced building blocks in the petrochemical industry,has received intense attention.Ethylene production,using electrochemical hydrogen pump-facilitated nonoxidative dehydrogenation of... Ethylene,one of the most widely produced building blocks in the petrochemical industry,has received intense attention.Ethylene production,using electrochemical hydrogen pump-facilitated nonoxidative dehydrogenation of ethane(NDE)to ethylene,is an emerging and promising route,promoting the transformation of the ethylene industry from energy-intensive steam cracking process to new electrochemical membrane reactor technology.In this work,the NDE reaction is incorporated into a BaZr_(0.1)Ce_(0.7)Y_(0.1)Yb_(0.1)O_(3-δ)electrolyte-supported protonic ceramic fuel cell membrane reactor to co-generate electricity and ethylene,utilizing the Nb and Cu doped perovskite oxide Pr_(0.6)Sr_(0.4)Fe_(0.8)Nb_(0.1)Cu_(0.1)O_(3-δ)(PSFNCu)as anode catalytic layer.Due to the doping of Nb and Cu,PSFNCu was endowed with high reduction tolerance and rich oxygen vacancies,showing excellent NDE catalytic performance.The maximum power density of the assembled reactor reaches 200 mW cm^(-2)at 750℃,with high ethane conversion(44.9%)and ethylene selectivity(92.7%).Moreover,the nitrous oxide decomposition was first coupled in the protonic ceramic fuel cell membrane reactor to consume the permeated protons.As a result,the generation of electricity,ethylene and decomposition of nitrous oxide can be simultaneously obtained by a single reactor.Specifically,the maximum power density of the cell reaches 208 mW cm^(-2)at 750℃,with high ethane conversion(45.2%),ethylene selectivity(92.5%),and nitrous oxide conversion(19,0%).This multi-win technology is promising for not only the production of chemicals and energy but also greenhouse gas reduction. 展开更多
关键词 Nonoxidative dehydrogenation of ethane ETHYLENE nitrous oxide decomposition Protonic ceramic fuel cell membrane reactor Perovskite oxide
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Influence of extra-framework Al in Fe-MOR catalysts for the direct conversion of methane to oxygenates by nitrous oxide 被引量:2
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作者 Shenglai Li Lisong Fan +2 位作者 Lina Song Dangguo Cheng Fengqiu Chen 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2021年第5期132-138,共7页
Iron-containing zeolites play an important role in the selective oxidation of methane to oxygenates by nitrous oxide.A solid-state ion exchange method is adopted to prepare Fe-MOR zeolite catalysts with different amou... Iron-containing zeolites play an important role in the selective oxidation of methane to oxygenates by nitrous oxide.A solid-state ion exchange method is adopted to prepare Fe-MOR zeolite catalysts with different amounts of extra-framework Al.EPR spectra and UV-vis spectra show that the percentage of iron ions in tetrahedral or octahedral coordination increases while those of clustered Fe species decrease by the addition of extra-framework Al species.Nitrous oxide titration reveals that more active Fe centers are formed,which promote the nitrous oxide consumption.The number of active centers in the catalyst with the introduction of extra-framework Al is about four times that of the catalyst without the addition of extra-framework Al.Due to this,there is an increase in the methane conversion,total selectivity and yield of oxygenates. 展开更多
关键词 Extra-framework AL METHANE conversion α-site nitrous oxide oxygenATES
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Built defects of homogeneous junction to enhance the lithium storage capacity of niobium pentoxide materials
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作者 Huibin Ding Yang Luo +5 位作者 Zihan Song Cong Chen Kai Feng Xiaofei Yang Hongzhang Zhang Xianfeng Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期730-737,共8页
Niobium pentoxide(Nb_(2)O_(5))is deemed one of the promising anode materials for lithium-ion batteries(LIBs)for its outstanding intrinsic fast Li-(de)intercalation kinetics.The specific capacity,however,is still limit... Niobium pentoxide(Nb_(2)O_(5))is deemed one of the promising anode materials for lithium-ion batteries(LIBs)for its outstanding intrinsic fast Li-(de)intercalation kinetics.The specific capacity,however,is still limited,because the(de)intercalation of excessive Li-ions brings the undesired stress to damage Nb_(2)O_(5) crystals.To increase the capacity of Nb_(2)O_(5) and alleviate the lattice distortion caused by stress,numerous homogeneous H-and M-phases junction interfaces were proposed to produce coercive stress within theNb_(2)O_(5)crystals.Such interfaces bring about rich oxygen vacancies with structural shrinkage tendency,which pre-generate coercive stress to resist the expansion stress caused by excessive Li-ions intercalation.Therefore,the synthesized Nb_(2)O_(5) achieves the highest lithium storage capacity of 315 mA h g−1 to date,and exhibits high-rate performance(118 mA h g^(-1) at 20 C)as well as excellent cycling stability(138 mA h g^(-1) at 10 C after 600 cycles). 展开更多
关键词 Niobiumpent oxide Homojunction polycrystalline DEFECTS oxygen vacancy
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Enhancing hydrogen evolution and oxidation kinetics through oxygen insertion into nickel lattice
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作者 Wanli Liang Xiyu Gong +9 位作者 Jinchang Xu Zixuan Dan Fanyan Xie Hulei Yu Hao-Fan Wang Yanshuo Jin Hongjuan Wang Yonghai Cao Hui Meng Hao Yu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期529-539,I0012,共12页
Nickel-based materials,including metallic Ni and Ni oxide,have been widely studied in the exploration of non-precious-metal hydrogen electrocatalysts,but neither pure Ni nor NiO is ideal for the hydrogen evolution rea... Nickel-based materials,including metallic Ni and Ni oxide,have been widely studied in the exploration of non-precious-metal hydrogen electrocatalysts,but neither pure Ni nor NiO is ideal for the hydrogen evolution reaction(HER)and hydrogen oxidation reaction(HOR).In this paper,an oxygen insertion strategy was applied on nickel to regulate its hydrogen electrocatalytic performance,and the oxygen-inserted nickel catalyst was successfully obtained with the assistance of tungsten dioxide support(denoted as O-Ni/WO_(2)).The partial insertion of oxygen in Ni maintains the face-centered cubic arrangement of Ni atoms,simultaneously expanding the lattice and increasing the lattice spacing.Consequently,the adsorption strength of^(*)H and^(*)OH on Ni is optimized,thus resulting in superior electrocatalytic performance of0-Ni/WO_(2)in alkaline HER/HOR.The Tafel slope of O-Ni/WO_(2)@NF for HER is 56 mV dec^(-1),and the kinetic current density of O-Ni/WO_(2)for HOR reaches 4.85 mA cm^(-2),which is ahead of most currently reported catalysts.Our proposed strategy of inserting an appropriate amount of anions into the metal lattice could provide more possibilities for the design of high-performance catalysts. 展开更多
关键词 Hydrogen evolution Hydrogen oxidation NICKEL oxygen insertion Adsorption free energy
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Designing Oxide Catalysts for Oxygen Electrocatalysis: Insights from Mechanism to Application 被引量:2
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作者 Ning Han Wei Zhang +7 位作者 Wei Guo Hui Pan Bo Jiang Lingbao Xing Hao Tian Guoxiu Wang Xuan Zhang Jan Fransaer 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第10期514-546,共33页
The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both hav... The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges. 展开更多
关键词 oxygen evolution oxygen reduction oxide catalysts Catalyst design Fuel cell Metal–air batteries
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Oxygen-defects evolution to stimulate continuous capacity increase in Co-free Li-rich layered oxides 被引量:2
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作者 Yibin Zhang Xiaohui Wen +3 位作者 Zhepu Shi Bao Qiu Guoxin Chen Zhaoping Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第7期259-267,I0006,共10页
Though oxygen defects are associated with deteriorated structures and aggravated cycling performance in traditional layered cathodes,the role of oxygen defects is still ambiguous in Li-rich layered oxides due to the i... Though oxygen defects are associated with deteriorated structures and aggravated cycling performance in traditional layered cathodes,the role of oxygen defects is still ambiguous in Li-rich layered oxides due to the involvement of oxygen redox.Herein,a Co-free Li-rich layered oxide Li_(1.286)Ni_(0.071)Mn_(0.643)O_(2)has been prepared by a co-precipitation method to systematically investigate the undefined effects of the oxygen defects.A significant O_(2)release and the propagation of oxygen vacancies were detected by operando differential electrochemical mass spectroscopy(DEMS)and electron energy loss spectroscopy(EELS),respectively.Scanning transmission electron microscopy-high angle annular dark field(STEMHAADF)reveals the oxygen vacancies fusing to nanovoids and monitors a stepwise electrochemical activation process of the large Li_(2)MnO_(3)domain upon cycling.Combined with the quantitative analysis conducted by the energy dispersive spectrometer(EDS),existed nano-scale oxygen defects actually expose more surface to the electrolyte for facilitating the electrochemical activation and subsequently increasing available capacity.Overall,this work persuasively elucidates the function of oxygen defects on oxygen redox in Co-free Li-rich layered oxides. 展开更多
关键词 Li-rich layered oxide Irreversible oxygen loss Nano-scale oxygen defect Li_(2)MnO_(3)-domain activation
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Ca and Sr co-doping induced oxygen vacancies in 3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts for boosting low-temperature oxidative coupling of methane
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作者 Tongtong Wu Yuechang Wei +5 位作者 Jing Xiong Yitao Yang Zhenpeng Wang Dawei Han Zhen Zhao Jian Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期331-344,共14页
It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(... It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(A_(2)B_(2)O_(7)-type)catalysts with disordered defective cubic fluorite phased structure were successfully prepared by a colloidal crystal template method.3DOM structure promotes the accessibility of the gaseous reactants(O2and CH4)to the active sites.The co-doping of Ca and Sr ions in La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts improved the formation of oxygen vacancies,thereby leading to increased density of surface-active oxygen species(O_(2)^(-))for the activation of CH4and the formation of C2products(C2H6and C2H4).3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts exhibit high catalytic activity for OCM at low temperature.3DOM La1.7Sr0.3Ce1.7Ca0.3O7-δcatalyst with the highest density of O_(2)^(-)species exhibited the highest catalytic activity for low-temperature OCM,i.e.,its CH4conversion,selectivity and yield of C2products at 650℃are 32.2%,66.1%and 21.3%,respectively.The mechanism was proposed that the increase in surface oxygen vacancies induced by the co-doping of Ca and Sr ions boosts the key step of C-H bond breaking and C-C bond coupling in catalyzing low-temperature OCM.It is meaningful for the development of the low-temperature and high-efficient catalysts for OCM reaction in practical application. 展开更多
关键词 3DOM catalysts Ca ions Sr ions Low-temperature oxidative couplingof methane oxygen vacancies O_(2)^(-) species
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Tuned d-band states over lanthanum doped nickel oxide for efficient oxygen evolution reaction 被引量:1
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作者 Ziyi Xiao Wei Zhou +7 位作者 Baopeng Yang Chengan Liao Qing Kang Gen Chen Min Liu Xiaohe Liu Renzhi Ma Ning Zhang 《Nano Materials Science》 EI CAS CSCD 2023年第2期228-236,共9页
The d-band state of materials is an important descriptor for activity of oxygen evolution reaction(OER).For NiO materials,there is rarely concern about tuning their d-band states to tailor the OER behaviors.Herein,NiO... The d-band state of materials is an important descriptor for activity of oxygen evolution reaction(OER).For NiO materials,there is rarely concern about tuning their d-band states to tailor the OER behaviors.Herein,NiO nanocrystals with doping small amount of La^(3+)were used to regulate d-band states for promoting OER activity.Density of states calculations based on density functional theory revealed that La^(3+)doping produced upper shift of d-band center,which would induce stronger electronic interaction between surface Ni atoms and species of oxygen evolution reaction intermediates.Further density functional theory calculation illustrated that La^(3+)doped NiO possessed reduced Gibbs free energy in adsorbing species of OER intermediate.Predicted by theoretical calculations,trace La^(3+)was introduced into crystal lattice of NiO nanoparticles.The La^(3+)doped NiO nanocrystal showed much promoted OER activity than corresponding pristine NiO product.Further electrochemical analysis revealed that La^(3+)doping into NiO increased the intrinsic activity such as improved active sites and reduced charge transfer resistance.The in-situ Raman spectra suggested that NiO phase in La^(3+)doped NiO could be better maintained than pristine NiO during the OER.This work provides an effective strategy to tune the d-band center of NiO for efficient electrocatalytic OER. 展开更多
关键词 Nickel oxide oxygen evolution reaction D-band center ELECTROCATALYSIS Water splitting
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Phase separation-hydrogen etching-derived Cu-decorated Cu-Mn bimetallic oxides with oxygen vacancies boosting superior sodium-ion storage kinetics 被引量:1
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作者 Lin Yan Lingshuo Zong +6 位作者 Qi Sun Junpeng Guo Zhenyang Yu Zhijun Qiao Jiuhui Han Zhenyu Cui Jianli Kang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第5期163-173,I0005,共12页
Understanding the crystal phase evolution of bimetallic oxide anodes is the main concern to profoundly reveal the conversion reaction kinetics and sodium-ion storage mechanisms.Herein,an integrated selfsupporting anod... Understanding the crystal phase evolution of bimetallic oxide anodes is the main concern to profoundly reveal the conversion reaction kinetics and sodium-ion storage mechanisms.Herein,an integrated selfsupporting anode of the Cu-decorated Cu-Mn bimetallic oxides with oxygen vacancies(Ov-BMO-Cu)are in-situ generated by phase separation and hydrogen etching using nanoporous Cu-Mn alloy as selfsacrificial templates.On this basis,we have elucidated the relationship between the phase evolution,oxygen vacancies and sodium-ion storage mechanisms,further demonstrating the evolution of oxygen vacancies and the inhibition effect of manganese oxides as an“anchor”on grain aggregation of copper oxides.The kinetic analyses confirm that the expanded lattice space and increased oxygen vacancies of cycled Ov-BMO-Cu synergistically guarantee effective sodium-ion diffusion and storage mechanisms.Therefore,the Ov-BMO-Cu electrode exhibits higher reversible capacities of 4.04 mA h cm^(-2)at 0.2 mA cm^(-2)after 100 cycles and 2.20 m A h cm^(-2)at 1.0 mA cm^(-2)after 500 cycles.Besides,the presodiated Ov-BMO-Cu anode delivers a considerable reversible capacity of 0.79 m A h cm^(-2)at 1.0 mA cm^(-2)after 60 cycles in full cells with Na_(3)V_(2)(PO_(4))_(3)cathode,confirming its outstanding practicality.Thus,this work is expected to provide enlightenment for designing high-capacity bimetallic oxide anodes. 展开更多
关键词 Sodium-ion storage mechanism Bimetallic oxide anode material Crystal phase evolution oxygen vacancies Kinetic analyses
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Rapid and durable oxygen reduction reaction enabled by a perovskite oxide with self-cleaning surface
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作者 Shengli Pang Yifan Song +7 位作者 Meng Cui Xin Tang Chao Long Lingfeng Ke Gongmei Yang Ting Fang Yong Guan Chonglin Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第8期333-340,I0010,共9页
The growth of electrochemically inert segregation layers on the surface of solid oxide fuel cell cathodes has become a bottleneck restricting the development of perovskite-structured oxygen reduction catalysts.Here,we... The growth of electrochemically inert segregation layers on the surface of solid oxide fuel cell cathodes has become a bottleneck restricting the development of perovskite-structured oxygen reduction catalysts.Here,we report a new discovery in which enriched Ba and Fe ions on the near-surface of Nd_(1/2)Ba_(1/2)Co_(1/3)Fe_(1/3)Mn_(1/3)O_(3-δ)spontaneously agglomerate into dispersed Ba_(5)Fe_(2)O_(8) nanoparticles and maintain a highly active and durable perovskite structure on the surface.This unique surface selfcleaning phenomenon is related to the low average potential energy of Ba_(5)Fe_(2)O_(8),which is grown on the near-surface layer.The electrochemically inert Ba_(5)Fe_(2)O_(8) segregation layer on the near-surface of the perovskite catalyst achieves self-cleaning by regulating the formation energy of enriched metal oxides.This self-cleaned perovskite surface exhibits an ultrafast oxygen exchange rate,high catalytic activity for the oxygen reduction reaction,and good adaptability to the actual working conditions of solid oxide fuel cell stacks.This study paves a new way for overcoming the stubborn problem of perovskite catalyst surface deactivation and enriches the scientific knowledge of surface catalysis. 展开更多
关键词 Surface chemistry Energy materials ELECTROCATALYSIS Perovskite oxide oxygen reduction reaction Solid oxide fuel cells
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Tuning the charge distribution and crystal field of iron single atoms via iron oxide integration for enhanced oxygen reduction reaction in zinc-air batteries
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作者 Feifei Zhang Yinlong Zhu +9 位作者 Yijun Zhong Jing Zou Yu Chen Lianhai Zu Zhouyou Wang Jack Jon Hinsch Yun Wang Lian Zhang Zongping Shao Huanting Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第10期154-163,I0006,共11页
Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged... Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged as attractive materials for potential replacement of Pt in ORR,but their catalytic performance was limited by the symmetrical electronic structure distribution around the single-atom Fe site.Here,we report our findings in significantly enhancing the ORR performance of Fe-N-C by moderate Fe_(2)O_(3) integration via the strong electronic interaction.Remarkably,the optimized catalyst(M-Fe_(2)O_(3)/Fe_(SA)@NC)exhibits excellent activity,durability and good tolerance to methanol,outperforming the benchmark Pt/C catalyst.When M-Fe_(2)O_(3)/Fe_(SA)@NC catalyst was used in a practical zinc-air battery assembly,peak power density of 155 mW cm^(-2)and specific capacity of 762 mA h g_(Zn)^(-1)were achieved and the battery assembly has shown superior cycling stability over a period of 200 h.More importantly,theoretical studies suggest that the introduction of Fe_(2)O_(3) can evoke the crystal field alteration and electron redistribution on single Fe atoms,which can break the symmetric charge distribution of Fe-N_(4) and thereby optimize the corresponding adsorption energy of intermediates to promote the O_(2)reduction.This study provides a new pathway to promote the catalytic performance of single-atom catalysts. 展开更多
关键词 Single-atom catalysts oxide nanoclusters Electronic interactions oxygen reduction reaction Zn-air battery
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Unexpected Li displacement and suppressed phase transition enabling highly stabilized oxygen redox in P3-type Na layered oxide cathode
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作者 Myungeun Choi Hobin Ahn +9 位作者 Hyunyoung Park Yongseok Lee Jinho Ahn Bonyoung Ku Junseong Kim Wonseok Ko Jungmin Kang Jung-Keun Yoo Duho Kim Jongsoon Kim 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第10期144-153,I0006,共11页
Oxygen redox is considered a new paradigm for increasing the practical capacity and energy density of the layered oxide cathodes for Na-ion batteries. However, severe local structural changes and phase transitions dur... Oxygen redox is considered a new paradigm for increasing the practical capacity and energy density of the layered oxide cathodes for Na-ion batteries. However, severe local structural changes and phase transitions during anionic redox reactions lead to poor electrochemical performance with sluggish kinetics.Here, we propose a synergy of Li-Cu cations in harnessing the full potential of oxygen redox, through Li displacement and suppressed phase transition in P3-type layered oxide cathode. P3-type Na_(0.7)[Li_(0.1)Cu_(0.2)Mn_(0.7)]O_(2) cathode delivers a large specific capacity of ~212 mA h g^(-1)at 15 mA g^(-1). The discharge capacity is maintained up to ~90% of the initial capacity after 100 cycles, with stable occurrence of the oxygen redox in the high-voltage region. Through advanced experimental analyses and first-principles calculations, it is confirmed that a stepwise redox reaction based on Cu and O ions occurs for the charge-compensation mechanism upon charging. Based on a concrete understanding of the reaction mechanism, the Li displacement by the synergy of Li-Cu cations plays a crucial role in suppressing the structural change of the P3-type layered material under the oxygen redox reaction, and it is expected to be an effective strategy for stabilizing the oxygen redox in the layered oxides of Na-ion batteries. 展开更多
关键词 Layered oxide cathode oxygen redox reaction Structural stability Li displacement No phase transition
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Nitrous oxide emission and reduction in a laboratory-incubated paddy soil response to pretreatment of water regime 被引量:14
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作者 WANGLian-feng CAIZu-cong YANHong 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2004年第3期353-357,共5页
A laboratory incubation experiment was conducted to investigate nitrous oxide(N 2O) emission and reduction in a paddy soil(Stagnic Anthrosol) response to the pretreatment of water regime. The paddy soil was maintaine... A laboratory incubation experiment was conducted to investigate nitrous oxide(N 2O) emission and reduction in a paddy soil(Stagnic Anthrosol) response to the pretreatment of water regime. The paddy soil was maintained under either air dried(sample D) or submerged(sample F) conditions for 110 d before the soil was adjusted into soil moisture of 20%, 40%, 60%, 80% and 100% water holding capacity(WHC) respectively, and then incubated with or without 10%(v/v) acetylene for 138 h at 25℃. At lower soil water content (≤60% WHC), N 2O emission from the sample F was 2 29 times higher than that from the sample D( P <0 01). While, N 2O emission from the sample F was only 29 and 14 percent of that from the sample D at the soil moisture of 80% and 100% WHC, respectively( P <0 01). The maximal N 2O emissions observed at soil moisture of 80% WHC were about 24 and 186 times higher than the minima obtained at the soil moisture of 20% WHC for the sample F and D, respectively. But at the soil moisture of 80% and 100% WHC, N 2O emission from the sample F with acetylene(F+ACE) was comparable to that of the sample D with acetylene (D+ACE). The results showed that the F sample produced N 2O ability in denitrification was similar to the sample D, however, the sample F was in the better reduction of N 2O to N 2 than the sample D even after the soil moisture was adjusted into the same level of 80% or 100% WHC. Therefore, the pretreatment of water regime influenced the strength and product composition of denitrification and N 2O emission from the paddy soil. 展开更多
关键词 DENITRIFICATION nitrous oxide reduction ACETYLENE product composition paddy soil
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Soil Nitrous Oxide Emissions Under Maize-Legume Intercropping System in the North China Plain 被引量:14
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作者 HUANG Jian-xiong CHEN Yuan-quan +2 位作者 SUI Peng NIE Sheng-wei GAO Wang-sheng 《Journal of Integrative Agriculture》 SCIE CAS CSCD 2014年第6期1363-1372,共10页
Many studies have focused on various agricultural management measures to reduce agricultural nitrous oxide (N2O) emission. However, few studies have investigated soil N2O emissions in intercropping systems in the No... Many studies have focused on various agricultural management measures to reduce agricultural nitrous oxide (N2O) emission. However, few studies have investigated soil N2O emissions in intercropping systems in the North China Plain. Thus, we conducted a ifeld experiment to compare N2O emissions under monoculture and maize-legume intercropping systems. In 2010, ifve treatments, including monocultured maize (M), maize-peanut (MP), maize-alfalfa (MA), maize-soybean (MS), and maize-sweet clover (MSC) intercropping were designed to investigate this issue using the static chamber technique. In 2011, M, MP, and MS remained, and monocultured peanuts (P) and soybean (S) were added to the trial. The results showed that total production of N2O from different treatments ranged from (0.87&#177;0.12) to (1.17&#177;0.11) kg ha-1 in 2010, while those ranged from (3.35&#177;0.30) to (9.10&#177;2.09) kg ha-1 in 2011. MA and MSC had no signiifcant effect on soil N2O production compared to that of M (P&lt;0.05). Cumulative N2O emissions from MP in 2010 were signiifcantly lower than those from M, but the result was the opposite in 2011 (P&lt;0.05). MS signiifcantly reduced soil N2O emissions by 25.55 and 48.84%in 2010 and 2011, respectively (P&lt;0.05). Soil N2O emissions were signiifcantly correlated with soil water content, soil temperature, nitriifcation potential, soil NH4+, and soil NO3-content (R2=0.160-0.764, P&lt;0.01). A stepwise linear regression analysis indicated that soil N2O release was mainly controlled by the interaction between soil moisture and soil NO3-content (R2=0.828, P&lt;0.001). These results indicate that MS had a coincident effect on soil N2O lfux and signiifcantly reduced soil N2O production compared to that of M over two growing seasons. 展开更多
关键词 MAIZE LEGUME INTERCROPPING soil nitrous oxide environmental factors
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Effects of Irrigation on Nitrous Oxide,Methane and Carbon Dioxide Fluxes in an Inner Mongolian Steppe 被引量:7
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作者 刘春岩 Jirko HOLST +5 位作者 Nicolas BRGGEMANN Klaus BUTTERBACH-BAHL 姚志生 韩圣慧 韩兴国 郑循华 《Advances in Atmospheric Sciences》 SCIE CAS CSCD 2008年第5期748-756,共9页
Increased precipitation during the vegetation periods was observed in and further predicted for Inner Mongolia. The changes in the associated soil moisture may affect the biosphere-atmosphere exchange of greenhouse ga... Increased precipitation during the vegetation periods was observed in and further predicted for Inner Mongolia. The changes in the associated soil moisture may affect the biosphere-atmosphere exchange of greenhouse gases. Therefore, we set up an irrigation experiment with one watered (W) and one unwatered plot (UW) at a winter-grazed Leymus chinensis-steppe site in the Xilin River catchment, Inner Mongolia. UW only received the natural precipitation of 2005 (129 mm), whereas W was additionally watered after the precipitation data of 1998 (in total 427 mm). In the 3-hour resolution, we determined nitrous oxide (N20), methane (CH4) and carbon dioxide (CO2) fluxes at both plots between May and September 2005, using a fully automated, chamber-based measuring system. N20 fluxes in the steppe were very low, with mean emissions (±s.e.) of 0.9-4-0.5 and 0.7-4-0.5 μg N m^-2 h^-1 at W and UW, respectively. The steppe soil always served as a CH4 sink, with mean fluxes of -24.1-4-3.9 and -31.1-4- 5.3 μg C m^-2 h^-1 at W and UW. Nighttime mean CO2 emissions were 82.6±8.7 and 26.3±1.7 mg C m^-2 h^-1 at W and UW, respectively, coinciding with an almost doubled aboveground plant biomass at W. Our results indicate that the ecosystem CO2 respiration responded sensitively to increased water input during the vegetation period, whereas the effects on CH4 and N2O fluxes were weak, most likely due to the high evapotranspiration and the lack of substrate for N2O producing processes. Based on our results, we hypothesize that with the gradual increase of summertime precipitation in Inner Mongolia, ecosystem CO2 respiration will be enhanced and CH4 uptake by the steppe soils will be lightly inhibited. 展开更多
关键词 nitrous oxide METHANE carbon dioxide semi-arid steppe IRRIGATION precipitation
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Pulmonary embolism and deep vein thrombosis caused by nitrous oxide abuse: A case report 被引量:8
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作者 Wen Sun Ji-Ping Liao +3 位作者 Yan Hu Wei Zhang Jing Ma Guang-Fa Wang 《World Journal of Clinical Cases》 SCIE 2019年第23期4057-4062,共6页
BACKGROUND Nitrous oxide(N2O)has gained increasing popularity as a recreational drug,causing hallucinations,excitation,and psychological dependence.However,side effects have been reported in recent years.Our case repo... BACKGROUND Nitrous oxide(N2O)has gained increasing popularity as a recreational drug,causing hallucinations,excitation,and psychological dependence.However,side effects have been reported in recent years.Our case report proposes a correlation among N2O,pulmonary embolism(PE),and deep vein thrombosis(DVT)and emphasizes the role of homocysteine(Hcy)in thrombotic events.CASE SUMMARY A 29-year-old man with long-term N2O abuse sought evaluation after acute chest pain.A diagnostic workup revealed PE,DVT,and hyperhomocysteinemia.The patient was successfully treated with thrombolytic and anticoagulant therapy.Moreover,his Hcy level decreased and returned to normal after Hcy-lowering therapy.CONCLUSION Chronic N2O abuse might increase the risk of PE and DVT,although there have been few studies previously. 展开更多
关键词 nitrous oxide Pulmonary EMBOLISM Deep VEIN THROMBOSIS HOMOCYSTEINE Case report
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Methane and Nitrous Oxide Emissions from Rice-Duck and Rice-Fish Complex Ecosystems and the Evaluation of Their Economic Significance 被引量:13
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作者 YUAN Wei-ling CAO Cou-gui LI Cheng-fang ZHAN Ming CAI Ming-li WANG Jin-ping 《Agricultural Sciences in China》 CAS CSCD 2009年第10期1246-1255,共10页
Rice-duck (RD) and rice-fish (RF) ecological systems are major complex planting and breeding models of rice paddy fields in southern China. Studying the methane (CH4) and nitrous oxide (N2O) emissions and thei... Rice-duck (RD) and rice-fish (RF) ecological systems are major complex planting and breeding models of rice paddy fields in southern China. Studying the methane (CH4) and nitrous oxide (N2O) emissions and their economic value from these two ecosystems can provide theoretical and practical basis for further development and utilization of these classical agricultural techniques. CH4 and N2O emissions from RD and RF ecological systems were measured in situ by using static chambers technique. Using global warming potentials (GWPs), we assessed the greenhouse effect of CH4 and N2O and their economic value. Results showed that the peaks of CH4 emission fluxes from RD and RF appeared at full tillering stage and at heading stage, and the average emission fluxes were significantly (P〈 0.05) lower than that from CK. N2O fluxes remained low when the field is flooded and high after draining the water. Compared with CK, the total amount of N2O emissions was significantly (P〈0.05) higher and slightly lower than those from RD and RF, respectively. In 2006 and 2007, the total greenhouse effect of CH4 and N20 from RD and RF were 4 728.3 and 4 611 kg CO2 ha^-1, 4 545 and 4 754.3 kg CO2 ha^-1, respectively. The costs of greenhouse effect were 970.89 and 946.81 RMB yuan ha^-1, and 933.25 and 976.23 RMB yuan ha^-1, respectively, which were significant lower than those from CK (5 997.6 and 5 391.5 RMB yuan ha^-1). Except for the environment cost of CH4 and N2O, the economic benefits from RD and RF were 2 210.64 and 4 881.92 RMB yuan ha^-1; 3 798.37 and 5 310.64 RMB yuan ha^-1, respectively, higher than those from CK. Therefore, RD and RF complex ecological planting and breeding models can effectively decrease and control CH4 and N2O emissions, and they are two of the effective strategies to reduce greenhouse gases from rice paddy fields and contribute in alleviating global warming. Thus, their adoption is important to the environment together with their economy benefits. 展开更多
关键词 methane emission nitrous oxide emission rice-duck complex ecosystem rice-fish complex ecosystem greenhouse effect economic benefit
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