Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silic...Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER catalyst.Compared to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@rGO.The CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)electrocatalyst.The achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their derivatives.The vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron density.Taking advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.展开更多
Charging P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)to 4.5 V for higher capacity is enticing.However,it leads to severe capacity fading,ascribing to the lattice oxygen evolution and the P2-O2 phase transformation.Here,the Mg Fe_...Charging P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)to 4.5 V for higher capacity is enticing.However,it leads to severe capacity fading,ascribing to the lattice oxygen evolution and the P2-O2 phase transformation.Here,the Mg Fe_(2)O_(4) coating and Mg,Fe co-doping were constructed simultaneously by Mg,Fe surface treatment to suppress lattice oxygen evolution and P2-O2 phase transformation of P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)at deep charging.Through ex-situ X-ray diffraction(XRD)tests,we found that the Mg,Fe bulk co-doping could reduce the repulsion between transition metals and Na+/vacancies ordering,thus inhibiting the P2-O2 phase transition and significantly reducing the irreversible volume change of the material.Meanwhile,the internal electric field formed by the dielectric polarization of Mg Fe_(2)O_(4) effectively inhibits the outward migration of oxidized O^(a-)(a<2),thereby suppressing the lattice oxygen evolution at deep charging,confirmed by in situ Raman and ex situ XPS techniques.P2-Na NM@MF-3 shows enhanced high-voltage cycling performance with capacity retentions of 84.8% and 81.3%at 0.1 and 1 C after cycles.This work sheds light on regulating the surface chemistry for Na-layered oxide materials to enhance the high-voltage performance of Na-ion batteries.展开更多
采用常规的固相反应法结合机械球磨制备了含碳质量分数23.7%的Li_(2)Ni_(2)(MoO_(4))3@C复合材料,并应用于锂离子电池负极。与纯Li_(2)Ni_(2)(MoO_(4))3相比,Li_(2)Ni_(2)(MoO_(4))3@C具有优异的电化学性能,在电流密度为200 mA ·g^...采用常规的固相反应法结合机械球磨制备了含碳质量分数23.7%的Li_(2)Ni_(2)(MoO_(4))3@C复合材料,并应用于锂离子电池负极。与纯Li_(2)Ni_(2)(MoO_(4))3相比,Li_(2)Ni_(2)(MoO_(4))3@C具有优异的电化学性能,在电流密度为200 mA ·g^(-1)时,50周循环后,可逆容量高达845 mAh·g^(-1)。值得注意的是,Li_(2)Ni_(2)(MoO_(4))3@C的首周库仑效率高达85%。此外,运用循环伏安法对Li_(2)Ni_(2)(MoO_(4))3@C复合物存储锂行为进行了初步探索。展开更多
Constructing the stable,low-cost,efficient,and highly adaptable visible light-driven photocatalyst to implement the synergistic effect of photocatalysis and adsorption has been excavated a promising strategy to deal w...Constructing the stable,low-cost,efficient,and highly adaptable visible light-driven photocatalyst to implement the synergistic effect of photocatalysis and adsorption has been excavated a promising strategy to deal with antibiotic pollution in water bodies.Herein,a novel 3 D ternary Z-scheme heterojunction photocatalyst Ni_(2)P/Bi_(2)MoO_(6)/g-C_(3)N_(4)(Ni_(2)P/BMO/CN)was fabricated by a simple solvothermal method in which the broad spectrum antibiotics(mainly tetracyclines and supplemented by quinolones)were used as target pollution sources to evaluate its adsorption and photocatalytic performance.Notably,the Zscheme composite significantly exhibit the enhancement for degradation efficiency of tetracycline and other antibiotic by using Ni_(2)P nanoparticles as electron conductor.Active species capture experiment and electron spin resonance(ESR)technology reveal the mechanism of Z-scheme Ni_(2)P/BMO/CN photocatalytic reaction in detail.In addition,based on the identification of intermediates by liquid chromatography–mass spectroscopy(LC–MS),the possible photocatalytic degradation pathways of TC were proposed.展开更多
Electrocatalytic CO_(2)reduction into CO has been regarded as one of the most promising strategies for sustainable carbon cycles at ambient conditions,but still faces challenges to achieve both high product selectivit...Electrocatalytic CO_(2)reduction into CO has been regarded as one of the most promising strategies for sustainable carbon cycles at ambient conditions,but still faces challenges to achieve both high product selectivity and large current density.Here,we report a Ni_(4)N/Ni_(3)ZnC_(0.7)heterostructured electrocatalyst embedded in accordion-like N-doped carbon through a simple molten salt annealing strategy.The optimal Ni_(4)N/Ni_(3)ZnC_(0.7)electrocatalyst achieves a high CO Faraday efficiency of 92.3%and a large total current density of-15.8 m A cm^(-2)at-0.8 V versus reversible hydrogen electrode,together with a long-term stability about 30 h.Density functional theory results reveal that the energy barrier for*COOH intermediate formation largely decreased on Ni_(4)N/Ni_(3)ZnC_(0.7)heterostructure compared with Ni_(4)N and Ni_(3)ZnC_(0.7),thus giving rise to enhanced activity and selectivity.A rechargeable Zn-CO_(2)battery is further assembled with Ni_(4)N/Ni_(3)ZnC_(0.7)catalyst as the cathode,which shows a maximum power density of 0.85 mW cm^(-2)and excellent stability.展开更多
Developing high performances aqueous rechargeable batteries is imperative and valuable.Herein,a novel aqueous rechargeable nickel//bismuth battery is developed based on highly porous Bi_(2)WO_(6) and Co_(0.5)Ni_(0.5)M...Developing high performances aqueous rechargeable batteries is imperative and valuable.Herein,a novel aqueous rechargeable nickel//bismuth battery is developed based on highly porous Bi_(2)WO_(6) and Co_(0.5)Ni_(0.5)MoO_(4) microspheres as electrode active materials.Porous Bi_(2)WO6 microspheres assembled from nanosheets as anode active materials can afford a specific capacity of179.2 mAh·g^(-1) at 1 A·g^(-1),rate capability of 74.7%in 1-20 A·g^(-1),and capacity retention of 57.2%for 1500 cycles at 15 A·g^(-1).Owing to the highly porous microsphere with’ribbon’-like and intertwined nanolayers morphology,the screened Co0.5Ni0.5MoO4 cathode active materials present an outstanding specific surface area of 293 m^(2)·g^(-1)and excellent electrochemical performance(such as superior specific capacity of 113.2 mAh·g^(-1) at 1 A·g^(-1),high rate performance of 51.8%in 1-15 A·g^(-1),and good capacity retention of 48.5%for 4600 cycles at15 A·g^(-1)).The corresponding aqueous rechargeable nickel//bismuth battery delivers the maximum energy density and power density of 35.8 Wh·kg^(-1) and3238.5 W·kg^(-1),respectively.The present research would offer a worthwhile guidance for the effective construction of electrode active materials for aqueous rechargeable nickel//bismuth batteries.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(DUT21LK34)Natural Science Foundation of Liaoning Province(2020-MS-113).
文摘Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER catalyst.Compared to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@rGO.The CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)electrocatalyst.The achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their derivatives.The vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron density.Taking advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.
基金supported by the Special Project for the Central Government to Guide Local Technological Development (GUIKE ZY20198008)the Guangxi Technology Base and talent Subject (GUIKE AD20238012,AD20297086)+5 种基金the Natural Science Foundation of Guangxi Province (2021GXNSFDA075012)the National Natural Science Foundation of China (51902108,52104298,22169004)the National Natural Science Foundation of China (U20A20249)the Regional Innovation and Development Joint Fundthe Guangxi Innovation Driven Development Subject (GUIKE AA19182020,19254004)the Special Fund for Guangxi Distinguished Expert。
文摘Charging P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)to 4.5 V for higher capacity is enticing.However,it leads to severe capacity fading,ascribing to the lattice oxygen evolution and the P2-O2 phase transformation.Here,the Mg Fe_(2)O_(4) coating and Mg,Fe co-doping were constructed simultaneously by Mg,Fe surface treatment to suppress lattice oxygen evolution and P2-O2 phase transformation of P2-Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)at deep charging.Through ex-situ X-ray diffraction(XRD)tests,we found that the Mg,Fe bulk co-doping could reduce the repulsion between transition metals and Na+/vacancies ordering,thus inhibiting the P2-O2 phase transition and significantly reducing the irreversible volume change of the material.Meanwhile,the internal electric field formed by the dielectric polarization of Mg Fe_(2)O_(4) effectively inhibits the outward migration of oxidized O^(a-)(a<2),thereby suppressing the lattice oxygen evolution at deep charging,confirmed by in situ Raman and ex situ XPS techniques.P2-Na NM@MF-3 shows enhanced high-voltage cycling performance with capacity retentions of 84.8% and 81.3%at 0.1 and 1 C after cycles.This work sheds light on regulating the surface chemistry for Na-layered oxide materials to enhance the high-voltage performance of Na-ion batteries.
基金supported by the National Natural Science Foundation of China(51871158)the Fundamental Research Program of Shanxi Province(201901D111273)+2 种基金the Innovation and Entrepreneurship Training Program for College Students of Shanxi Province(20210491)Scientific and technological innovation project of colleges and universities in Shanxi Province(2020L0353)the PhD Startup Fund of Taiyuan University of Science and Technology(20182003).
文摘采用常规的固相反应法结合机械球磨制备了含碳质量分数23.7%的Li_(2)Ni_(2)(MoO_(4))3@C复合材料,并应用于锂离子电池负极。与纯Li_(2)Ni_(2)(MoO_(4))3相比,Li_(2)Ni_(2)(MoO_(4))3@C具有优异的电化学性能,在电流密度为200 mA ·g^(-1)时,50周循环后,可逆容量高达845 mAh·g^(-1)。值得注意的是,Li_(2)Ni_(2)(MoO_(4))3@C的首周库仑效率高达85%。此外,运用循环伏安法对Li_(2)Ni_(2)(MoO_(4))3@C复合物存储锂行为进行了初步探索。
基金financially supported by the National Natural Science Foundation of China(No.21906072,22006057,21671084 and 51902140)the Natural Science Foundation of Jiangsu Province(BK20190982)+2 种基金Henan Postdoctoral Foundation(202003013)“Doctor of Mass entrepreneurship and innovation”Project in Jiangsu Province,Jiangsu 333 talents project funding(BRA2018342)Jiangsu provincial government scholarship for overseas studies,the Doctoral Scientific Research Foundation of Jiangsu University of Science and Technology(China)(1062931806 and 1142931803)。
文摘Constructing the stable,low-cost,efficient,and highly adaptable visible light-driven photocatalyst to implement the synergistic effect of photocatalysis and adsorption has been excavated a promising strategy to deal with antibiotic pollution in water bodies.Herein,a novel 3 D ternary Z-scheme heterojunction photocatalyst Ni_(2)P/Bi_(2)MoO_(6)/g-C_(3)N_(4)(Ni_(2)P/BMO/CN)was fabricated by a simple solvothermal method in which the broad spectrum antibiotics(mainly tetracyclines and supplemented by quinolones)were used as target pollution sources to evaluate its adsorption and photocatalytic performance.Notably,the Zscheme composite significantly exhibit the enhancement for degradation efficiency of tetracycline and other antibiotic by using Ni_(2)P nanoparticles as electron conductor.Active species capture experiment and electron spin resonance(ESR)technology reveal the mechanism of Z-scheme Ni_(2)P/BMO/CN photocatalytic reaction in detail.In addition,based on the identification of intermediates by liquid chromatography–mass spectroscopy(LC–MS),the possible photocatalytic degradation pathways of TC were proposed.
基金financially supported by the National Key Research and Development Program,China(2018YFB1502503)the 2021 Talent Introduction Project of Chongqing Medical and Pharmaceutical College(ygz2021104)。
文摘Electrocatalytic CO_(2)reduction into CO has been regarded as one of the most promising strategies for sustainable carbon cycles at ambient conditions,but still faces challenges to achieve both high product selectivity and large current density.Here,we report a Ni_(4)N/Ni_(3)ZnC_(0.7)heterostructured electrocatalyst embedded in accordion-like N-doped carbon through a simple molten salt annealing strategy.The optimal Ni_(4)N/Ni_(3)ZnC_(0.7)electrocatalyst achieves a high CO Faraday efficiency of 92.3%and a large total current density of-15.8 m A cm^(-2)at-0.8 V versus reversible hydrogen electrode,together with a long-term stability about 30 h.Density functional theory results reveal that the energy barrier for*COOH intermediate formation largely decreased on Ni_(4)N/Ni_(3)ZnC_(0.7)heterostructure compared with Ni_(4)N and Ni_(3)ZnC_(0.7),thus giving rise to enhanced activity and selectivity.A rechargeable Zn-CO_(2)battery is further assembled with Ni_(4)N/Ni_(3)ZnC_(0.7)catalyst as the cathode,which shows a maximum power density of 0.85 mW cm^(-2)and excellent stability.
基金financially supported by the National Natural Science Foundation of China(Nos.21374016 and 21304018)Jiangsu Provincial Natural Science Foundation of China(Nos.BK20130619 and BK20130617)+1 种基金the Scientific and Technological Project of Henan Province(No.222102240092)the fundamental Research Funds for the Central Universities。
文摘Developing high performances aqueous rechargeable batteries is imperative and valuable.Herein,a novel aqueous rechargeable nickel//bismuth battery is developed based on highly porous Bi_(2)WO_(6) and Co_(0.5)Ni_(0.5)MoO_(4) microspheres as electrode active materials.Porous Bi_(2)WO6 microspheres assembled from nanosheets as anode active materials can afford a specific capacity of179.2 mAh·g^(-1) at 1 A·g^(-1),rate capability of 74.7%in 1-20 A·g^(-1),and capacity retention of 57.2%for 1500 cycles at 15 A·g^(-1).Owing to the highly porous microsphere with’ribbon’-like and intertwined nanolayers morphology,the screened Co0.5Ni0.5MoO4 cathode active materials present an outstanding specific surface area of 293 m^(2)·g^(-1)and excellent electrochemical performance(such as superior specific capacity of 113.2 mAh·g^(-1) at 1 A·g^(-1),high rate performance of 51.8%in 1-15 A·g^(-1),and good capacity retention of 48.5%for 4600 cycles at15 A·g^(-1)).The corresponding aqueous rechargeable nickel//bismuth battery delivers the maximum energy density and power density of 35.8 Wh·kg^(-1) and3238.5 W·kg^(-1),respectively.The present research would offer a worthwhile guidance for the effective construction of electrode active materials for aqueous rechargeable nickel//bismuth batteries.
