Rational design of low-cost, highly electrocatalytic activity, and stable bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) has been a great significant for metal–air...Rational design of low-cost, highly electrocatalytic activity, and stable bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) has been a great significant for metal–air batteries. Herein, an efficient bifunctional electrocatalyst based on hollow cobalt oxide nanoparticles embedded in nitrogen-doped carbon nanosheets(Co/N-Pg) is fabricated for Zn–air batteries. A lowcost biomass peach gum, consisting of carbon, oxygen, and hydrogen without other heteroatoms, was used as carbon source to form carbon matrix hosting hollow cobalt oxide nanoparticles. Meanwhile, the melamine was applied as nitrogen source and template precursor, which can convert to carbon-based template graphitic carbon nitride by polycondensation process. Owing to the unique structure and synergistic effect between hollow cobalt oxide nanoparticles and Co-N-C species, the proposal Co/N-Pg catalyst displays not only prominent bifunctional electrocatalytic activities for ORR and OER, but also excellent durability. Remarkably, the assembled Zn–air battery with Co/N-Pg air electrode exhibited a low discharge-charge voltage gap(0.81 V at 50 mA cm^-2) and high peak power density(119 mW cm^-2) with long-term cycling stability. This work presents an effective approach for engineering transition metal oxides and nitrogen modified carbon nanosheets to boost the performance of bifunctional electrocatalysts for Zn–air battery.展开更多
Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are crucial for the large-scale application of rech...Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are crucial for the large-scale application of rechargeable Zn-air batteries(ZABs).In this work,our density functional theory calculations on the electrocatalyst suggest that the rational construction of interfacial structure can induce local charge redistribution,improve the electronic conductivity and enhance the catalyst stability.In order to realize such a structure,we spatially immobilize heterogeneous CoS/CoO nanocrystals onto N-doped graphene to synthesize a bifunctional electrocatalyst(CoS/CoO@NGNs).The optimization of the composition,interfacial structure and conductivity of the electrocatalyst is conducted to achieve bifunctional catalytic activity and deliver outstanding efficiency and stability for both ORR and OER.The aqueous ZAB with the as-prepared CoS/CoO@NGNs cathode displays a high maximum power density of 137.8 mW cm^−2,a specific capacity of 723.9 mAh g^−1 and excellent cycling stability(continuous operating for 100 h)with a high round-trip efficiency.In addition,the assembled quasi-solid-state ZAB also exhibits outstanding mechanical flexibility besides high battery performances,showing great potential for applications in flexible and wearable electronic devices.展开更多
In the original publication,the label text“Pt/C”in Fig.5 should be“Pt/C+IrO_(2)”.In Fig.5d,the X-axis label“Poten-tial(V vs.RHE)”should be replaced with“Specific capacity(mAh g^(−1))”.In Fig.5e,the Y-axis labe...In the original publication,the label text“Pt/C”in Fig.5 should be“Pt/C+IrO_(2)”.In Fig.5d,the X-axis label“Poten-tial(V vs.RHE)”should be replaced with“Specific capacity(mAh g^(−1))”.In Fig.5e,the Y-axis label“Potential(V vs.RHE)”should be replaced with“Voltage(V)”.In Fig.5g,the X-axis label“Time(h)”should be replaced with“Cycle number(n)”.The Y-axis label“ΔE(V vs.RHE)”should be replaced with“Voltage(V)”.The number“1.4”and“1.6”should be replaced with 1.6 and 2.0,respectively.The cor-responding data analysis and conclusions in the manuscript are not affected and thus not to be changed.The correct Fig.5 is provided in this correction.展开更多
Black phosphorus(BP),an interesting and multi-functional non-metal material,has attracted widespread attention.In this work,2D BP/2D g-C3N4 heterostructure had been fabricated at extremely low temperature,which was us...Black phosphorus(BP),an interesting and multi-functional non-metal material,has attracted widespread attention.In this work,2D BP/2D g-C3N4 heterostructure had been fabricated at extremely low temperature,which was used to reduce CO2 for the first time.With introduction of 2D BP,the separation of photogenerated holes and electrons was extremely boosted,and composites showed excellent photocatalytic performance(CO2 to CO).Meanwhile,the targeted composite could keep high selectivity for CO generation and CO generation rate can be up to 187.7μmol g−1 h^−1.The formation process of the unique heterostructure and the key factor affecting the photocatalytic performance were also discussed.This work provides a new approach for designing metal free photocatalyst,which is used for CO2 reduction.展开更多
Due to the poor Fenton reactivity,single-atom Mn-based materials are generally identified as one of the most promising active catalysts for oxygen reduction reaction(ORR).Regulating the electronic density and coordina...Due to the poor Fenton reactivity,single-atom Mn-based materials are generally identified as one of the most promising active catalysts for oxygen reduction reaction(ORR).Regulating the electronic density and coordination environment of atomically dispersed Mn centers is an effective strategy to enhance ORR activity of Mn-based materials.By introducing Zn sites,atomically dispersed Mn centers with multitudes of coordination(including Zn/Mn–Nx and Mn–Nx moieties)can be constructed to form Mn-based ORR catalyst(Zn/Mn-NC)with dual-atom sites.Around Mn–Nx sites,the Zn atoms can effectively modulate the electronic structure and coordination state of Mn centers in Zn/Mn-NC through d–d orbital coupling.The electronic interaction between Zn and Mn sites improves ORR activity,thereby optimizing the oxygen adsorption energy of Mn sites in Zn/Mn-NC and reducing the overall energy barrier.Zn/Mn-NC displays higher ORR half-wave potential than Pt/C(0.89 V vs 0.86 V).The quasi-solid-state zinc-air battery(ZAB)with Zn/Mn-NC as the cathode displayed excellent rechargeability,recyclability,and mechanical robustness.The strategy presented regulates the electronic density and coordination environment of singleatom Mn-based ORR catalysts in quasi-solid-state ZABs.展开更多
On the basis of hydrothermal synthesis of Ag-CeO2 microspheres,Ag-CeO2/g-C3N4 composite photocatalyst with heterostructure was prepared by simple solvent evaporation of Ag-CeO2 and g-C3N4.To characterize the compositi...On the basis of hydrothermal synthesis of Ag-CeO2 microspheres,Ag-CeO2/g-C3N4 composite photocatalyst with heterostructure was prepared by simple solvent evaporation of Ag-CeO2 and g-C3N4.To characterize the composition,structure,morphology and light absorption properties of the as-prepared Ag-CeO2/g-C3N4 composites,XRD,FTIR XPS,SEM,TEM,PL,BET and UV-vis DRS were used,respectively.The as-prepared photocatalyst was subjected to photocatalytic degradation of pollutants,and the prepared composite material has excellent photocatalytic activity for photodegradation of methylene blue(MB).The research shows that the photocatalytic properties of Ag-CeO2/g-C3N4 composites were related to the mass ratio of Ag-CeO2 microspheres and g-C3N4 nanosheets.When the ratio of Ag-CeO2 microspheres:g-C3N4 is 1:5,the composites have the highest photocatalytic activity,which was 9.6 and 3.3 times that of single Ag-CeO2 and g-C3N4,respectively.The improvement of photocatalytic activity is attributed to the heterostructure between the composite materials and the addition of noble metal silver,and the degradation of methylene blue by the visible light irradiation material is greatly improved.Finally,an attempt was made to analyze the principle of photocatalytic degradation of pollutants in prepared materials.展开更多
Hierarchically hollow nanostructures have been the focus of numerous studies due to their prominent physicochemical properties that differ significantly from bulk materials and their potential for extensive applicatio...Hierarchically hollow nanostructures have been the focus of numerous studies due to their prominent physicochemical properties that differ significantly from bulk materials and their potential for extensive applications. We present a novel diatom-based scaffold for the synthesis of hierarchically biomorphic CeO2 with special porous structure via incorporating Ce ions into the frustule.Scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and nitrogen adsorption-desorption measurements were adopted to characterize the products. Owing to its unique hierarchical structure and periodic meso-macro scale features, the obtained CeO2 exhibits high catalytic activity in CO oxidation. This facile strategy may design a new way towards replicating desired biological structures for metal oxide catalyst in other potential applications.展开更多
Cerium fluoride(CeF_(3))semiconductor with upconversion property was constructed on graphite carbonitride(g-C_(3) N_(4))nanosheets by microwave hydrothermal method.The X-ray diffraction,transmission election microscop...Cerium fluoride(CeF_(3))semiconductor with upconversion property was constructed on graphite carbonitride(g-C_(3) N_(4))nanosheets by microwave hydrothermal method.The X-ray diffraction,transmission election microscopy,Fourier transform infrared,and X-ray photoelectron spectra techniques were used to characterize the CeF_(3)/g-C_(3)N_(4) nanocomposite.The study shows that CeF_(3) has upconversion property and can convert visible light(Vis)and near-infrared light(NIR)into ultraviolet light(UV).Mo reover,CeF3 and g-C_(3) N_(4) can form well-defined heterojunction and promote the effective separation of photogenerated electrons and holes.The synergistic effect of the CeF_(3)/g-C_(3)N_(4) nanocomposite was evaluated by photocatalytic degradation of dibenzothiophene(DBT).The optimum photocatalyst of CeF_(3)/g-C_(3)N_(4)(40 wt%)composites exhibit the highest photocatalytic desulfurization rate of the model oil under visible light radiation.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos. 21506081, 21705058, 21676126)the Provincial Natural Science Foundation of Jiangsu (Nos. BK20170524, BK20160492)+2 种基金China Postdoctoral Science Foundation (No. 2018T110450)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education InstitutionsThe financial support from an ARC Discovery Project (No. DP180102003)
文摘Rational design of low-cost, highly electrocatalytic activity, and stable bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) has been a great significant for metal–air batteries. Herein, an efficient bifunctional electrocatalyst based on hollow cobalt oxide nanoparticles embedded in nitrogen-doped carbon nanosheets(Co/N-Pg) is fabricated for Zn–air batteries. A lowcost biomass peach gum, consisting of carbon, oxygen, and hydrogen without other heteroatoms, was used as carbon source to form carbon matrix hosting hollow cobalt oxide nanoparticles. Meanwhile, the melamine was applied as nitrogen source and template precursor, which can convert to carbon-based template graphitic carbon nitride by polycondensation process. Owing to the unique structure and synergistic effect between hollow cobalt oxide nanoparticles and Co-N-C species, the proposal Co/N-Pg catalyst displays not only prominent bifunctional electrocatalytic activities for ORR and OER, but also excellent durability. Remarkably, the assembled Zn–air battery with Co/N-Pg air electrode exhibited a low discharge-charge voltage gap(0.81 V at 50 mA cm^-2) and high peak power density(119 mW cm^-2) with long-term cycling stability. This work presents an effective approach for engineering transition metal oxides and nitrogen modified carbon nanosheets to boost the performance of bifunctional electrocatalysts for Zn–air battery.
基金the National Natural Science Foundation of China(Grant Numbers 21506081)the Provincial Natural Science Foundation of Jiangsu(Grant Numbers BK20191430)+2 种基金Six Talent Peaks Project of Jiangsu Province[Grant Numbers XNY-009]High-tech research key laboratory of Zhenjiang(Grant Numbers SS2018002)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions and the Research Foundation of Jiangsu University(Grant Numbers 17JDG007).
文摘Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are crucial for the large-scale application of rechargeable Zn-air batteries(ZABs).In this work,our density functional theory calculations on the electrocatalyst suggest that the rational construction of interfacial structure can induce local charge redistribution,improve the electronic conductivity and enhance the catalyst stability.In order to realize such a structure,we spatially immobilize heterogeneous CoS/CoO nanocrystals onto N-doped graphene to synthesize a bifunctional electrocatalyst(CoS/CoO@NGNs).The optimization of the composition,interfacial structure and conductivity of the electrocatalyst is conducted to achieve bifunctional catalytic activity and deliver outstanding efficiency and stability for both ORR and OER.The aqueous ZAB with the as-prepared CoS/CoO@NGNs cathode displays a high maximum power density of 137.8 mW cm^−2,a specific capacity of 723.9 mAh g^−1 and excellent cycling stability(continuous operating for 100 h)with a high round-trip efficiency.In addition,the assembled quasi-solid-state ZAB also exhibits outstanding mechanical flexibility besides high battery performances,showing great potential for applications in flexible and wearable electronic devices.
文摘In the original publication,the label text“Pt/C”in Fig.5 should be“Pt/C+IrO_(2)”.In Fig.5d,the X-axis label“Poten-tial(V vs.RHE)”should be replaced with“Specific capacity(mAh g^(−1))”.In Fig.5e,the Y-axis label“Potential(V vs.RHE)”should be replaced with“Voltage(V)”.In Fig.5g,the X-axis label“Time(h)”should be replaced with“Cycle number(n)”.The Y-axis label“ΔE(V vs.RHE)”should be replaced with“Voltage(V)”.The number“1.4”and“1.6”should be replaced with 1.6 and 2.0,respectively.The cor-responding data analysis and conclusions in the manuscript are not affected and thus not to be changed.The correct Fig.5 is provided in this correction.
基金supported by the National Natural Science Foundation of China(21676128,21776118,51902138)Hightech Research Key laboratory of Zhenjiang(SS2018002)+4 种基金Jiangsu Funds for Distinguished Young Scientists(BK20190045)Natural Science Foundation of Jiangsu Province(BK20190835)the Priority Academic Program Development of Jiangsu Higher Education Institutions,Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province(KFKT2019002)Construction funding of High-level teachers,Jiangsu University(4111510008)the High Performance Computing Platform of Jiangsu University.
文摘Black phosphorus(BP),an interesting and multi-functional non-metal material,has attracted widespread attention.In this work,2D BP/2D g-C3N4 heterostructure had been fabricated at extremely low temperature,which was used to reduce CO2 for the first time.With introduction of 2D BP,the separation of photogenerated holes and electrons was extremely boosted,and composites showed excellent photocatalytic performance(CO2 to CO).Meanwhile,the targeted composite could keep high selectivity for CO generation and CO generation rate can be up to 187.7μmol g−1 h^−1.The formation process of the unique heterostructure and the key factor affecting the photocatalytic performance were also discussed.This work provides a new approach for designing metal free photocatalyst,which is used for CO2 reduction.
基金support of the National Natural Science Foundation of China(grant nos.22278193 and 22178148)Jiangsu Province and Education Ministry Cosponsored Synergistic Innovation Center of Modern Agricultural Equipment(grant no.XTCX2029)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Due to the poor Fenton reactivity,single-atom Mn-based materials are generally identified as one of the most promising active catalysts for oxygen reduction reaction(ORR).Regulating the electronic density and coordination environment of atomically dispersed Mn centers is an effective strategy to enhance ORR activity of Mn-based materials.By introducing Zn sites,atomically dispersed Mn centers with multitudes of coordination(including Zn/Mn–Nx and Mn–Nx moieties)can be constructed to form Mn-based ORR catalyst(Zn/Mn-NC)with dual-atom sites.Around Mn–Nx sites,the Zn atoms can effectively modulate the electronic structure and coordination state of Mn centers in Zn/Mn-NC through d–d orbital coupling.The electronic interaction between Zn and Mn sites improves ORR activity,thereby optimizing the oxygen adsorption energy of Mn sites in Zn/Mn-NC and reducing the overall energy barrier.Zn/Mn-NC displays higher ORR half-wave potential than Pt/C(0.89 V vs 0.86 V).The quasi-solid-state zinc-air battery(ZAB)with Zn/Mn-NC as the cathode displayed excellent rechargeability,recyclability,and mechanical robustness.The strategy presented regulates the electronic density and coordination environment of singleatom Mn-based ORR catalysts in quasi-solid-state ZABs.
基金supported by the National Key R&D Program of China(2021YFA1600202)the National Natural Science Foundation of China(U2032162,81972191,U1932158,and 81871085)+7 种基金Hefei Institutes of Physical Science Director’s Fund(BJPY2021B06)the Collaborative Innovation Program of Hefei Science Center of CAS(2022HSCCIP013)Anhui Provincial Natural Science Foundation(2208085J10)Hefei Municipal Natural Science Foundation(2021009)the Natural Science Foundation of Shandong Province(ZR2019LZL018)the High Magnetic Field Laboratory of Anhui Province(AHHM-FX-2021-04)the Project of China Postdoctoral Science Foundation(2019M652403)the Project of Postdoctoral Innovation of Shandong Province(202002048)。
基金Project supported by the National Natural Science Foundation of China(51478285,21407111)Natural Science Foundation of Jiangsu Province(BK20180971,BK20180103)
文摘On the basis of hydrothermal synthesis of Ag-CeO2 microspheres,Ag-CeO2/g-C3N4 composite photocatalyst with heterostructure was prepared by simple solvent evaporation of Ag-CeO2 and g-C3N4.To characterize the composition,structure,morphology and light absorption properties of the as-prepared Ag-CeO2/g-C3N4 composites,XRD,FTIR XPS,SEM,TEM,PL,BET and UV-vis DRS were used,respectively.The as-prepared photocatalyst was subjected to photocatalytic degradation of pollutants,and the prepared composite material has excellent photocatalytic activity for photodegradation of methylene blue(MB).The research shows that the photocatalytic properties of Ag-CeO2/g-C3N4 composites were related to the mass ratio of Ag-CeO2 microspheres and g-C3N4 nanosheets.When the ratio of Ag-CeO2 microspheres:g-C3N4 is 1:5,the composites have the highest photocatalytic activity,which was 9.6 and 3.3 times that of single Ag-CeO2 and g-C3N4,respectively.The improvement of photocatalytic activity is attributed to the heterostructure between the composite materials and the addition of noble metal silver,and the degradation of methylene blue by the visible light irradiation material is greatly improved.Finally,an attempt was made to analyze the principle of photocatalytic degradation of pollutants in prepared materials.
基金supported by the National Natural Science Foundation of China (21071107, 21277094, 21103119)Production and Research Collaborative Innovation Project of Jiangsu Province (BY2012123)+6 种基金Natural Science Foundation of Jiangsu Province (BK2012167)Science and Technology Pillar Program (Industry) of Jiangsu Province (BE2012101)Collegiate Natural Science Fund of Jiangsu Province (12KJA430005, 11KJB430012)Jiangsu Key Laboratory for Photon Manufacturing (GZ201111)Jiangsu Provincial Key Laboratory for Interventional Medical Devices (Jr1210)Science and Technology Pillar Program (Industry) of Changzhou (CE20120067)Creative Project of Postgraduate of Jiangsu Province(CXLX12_0635).
文摘Hierarchically hollow nanostructures have been the focus of numerous studies due to their prominent physicochemical properties that differ significantly from bulk materials and their potential for extensive applications. We present a novel diatom-based scaffold for the synthesis of hierarchically biomorphic CeO2 with special porous structure via incorporating Ce ions into the frustule.Scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and nitrogen adsorption-desorption measurements were adopted to characterize the products. Owing to its unique hierarchical structure and periodic meso-macro scale features, the obtained CeO2 exhibits high catalytic activity in CO oxidation. This facile strategy may design a new way towards replicating desired biological structures for metal oxide catalyst in other potential applications.
基金supported by the National Natural Science Foundation of China(11774178,51801172)the Jiangsu Province Key Laboratory of Materials Surface Science and Technology and School-level Research Projects of Yancheng Institute of Technology(xjr2019026)。
文摘Cerium fluoride(CeF_(3))semiconductor with upconversion property was constructed on graphite carbonitride(g-C_(3) N_(4))nanosheets by microwave hydrothermal method.The X-ray diffraction,transmission election microscopy,Fourier transform infrared,and X-ray photoelectron spectra techniques were used to characterize the CeF_(3)/g-C_(3)N_(4) nanocomposite.The study shows that CeF_(3) has upconversion property and can convert visible light(Vis)and near-infrared light(NIR)into ultraviolet light(UV).Mo reover,CeF3 and g-C_(3) N_(4) can form well-defined heterojunction and promote the effective separation of photogenerated electrons and holes.The synergistic effect of the CeF_(3)/g-C_(3)N_(4) nanocomposite was evaluated by photocatalytic degradation of dibenzothiophene(DBT).The optimum photocatalyst of CeF_(3)/g-C_(3)N_(4)(40 wt%)composites exhibit the highest photocatalytic desulfurization rate of the model oil under visible light radiation.