As a catalyst of the air cathode in zinc-air batteries,tungstic acid ferrous(FeWO_(4)),a nanoscale transition metal tungstate,shows a broad application prospect in the oxygen reduction reaction(ORR).While FeWO_(4)poss...As a catalyst of the air cathode in zinc-air batteries,tungstic acid ferrous(FeWO_(4)),a nanoscale transition metal tungstate,shows a broad application prospect in the oxygen reduction reaction(ORR).While FeWO_(4)possesses favorable electrochemical properties and thermodynamic stability,its intrinsic semiconductor characteristics result in a relatively slow electron transfer rate,limiting the ORR catalytic activity.In this work,the electronic structure of FeWO_(4)is significantly modulated by introducing phosphorus(P)atoms with abundant valence electrons.The P doping can adjust the electronic structure of FeWO_(4)and then optimize oxygen-containing intermediates'absorption/desorption efficiency to achieve improved ORR activity.Furthermore,the sodium chloride template is utilized to construct a porous carbon framework for anchoring phosphorus-doped iron tungstate(P-FeWO_(4)/PNC).The porous carbon skeleton provides numerous active sites for the absorption/desorption and redox reactions on the P-FeWO_(4)/PNC surface and serves as mass transport channels for reactants and intermediates.The P-FeWO_(4)/PNC demonstrates ORR performance(E1/2=0.86 V vs.RHE).Furthermore,the zinc-air batteries incorporating the P-FeWO_(4)/PNC composite demonstrate an increased peak power density(172.2 mW·cm^(-2)),high specific capacity(810.1 mAh·g^(-1)),and sustained long-term cycling stability lasting up to 240 h.This research not only contributes to the advancement of cost-effective tungsten-based non-precious metallic ORR catalysts,but also guides their utilization in zinc-air batteries.展开更多
Poly(3-hexylthiophene)(P3HT)is one of the most promising hole-transporting materials in the pursuit of efficient and stable perovskite solar cells due to its outstanding stability and low cost.However,the intrinsic lo...Poly(3-hexylthiophene)(P3HT)is one of the most promising hole-transporting materials in the pursuit of efficient and stable perovskite solar cells due to its outstanding stability and low cost.However,the intrinsic low carrier density of P3 HT and poor contact between the P3HT/perovskite interface always lead to a low performance of the solar cell,while conventional chemical doping always makes the films unstable and limits the scalability.In this work,for the first time,we simultaneously enhanced the hole transporting properties of P3HT film and the interface of perovskite by doping it with a judiciously designed oxidized small molecule organic semiconductor.The organic salt not only can promote the lamellar crystallinity of P3HT to obtain better charge transport properties,but also reduce the defects of perovskite.As a result,we achieved champion efficiencies of 23.0%for small-area solar cells and 18.8%for larger-area modules(48.0 cm^(2)).This efficiency is the highest value for P3HT-based perovskite modules.Moreover,the solar cells show excellent operational stability,retaining over 95%of their initial efficiencies after1200 h of continuous operation.展开更多
Traditional photo-electcatalyst structures of small noble metal nanoparticles assembling into large-scale photoactive semiconductors still suffer from agglomeration of noble metal nanoparticles,insufficient charge tra...Traditional photo-electcatalyst structures of small noble metal nanoparticles assembling into large-scale photoactive semiconductors still suffer from agglomeration of noble metal nanoparticles,insufficient charge transfer,undesirable photoresponse ability that restricted the photo-electrocatalytic performance.To this end,a novel design strategy is proposed in this work,namely integrating small-scale photoactive materials(doped graphene quantum dots,S,N-GQDs)with large-sized noble metal(Pd P)nanoflowers to form novel photo-electrocatalysts for high-efficient alcohol oxidation reaction.As expected,superior electrocatalytic performance of Pd P/S,N-GQDs for ethylene glycol oxidation is acquired,thanks to the nanoflower structure with larger specific surface area and abundant active sites.Furthermore,nonmetal P are demonstrated,especially optimizing the adsorption strength,enhancing the interfacial contact,reducing metal agglomeration,ensuring uniform and efficient doping of S,N-GQDs,and ultimately significantly boost the catalytic activity of photo-electrocatalysts.展开更多
Stimulated emission and lasing of GaN-based laser diodes(LDs)were reported at 1995[1]and 1996[2],right after the breakthrough of p-type doping[3−5],material quality[6]and the invention of high-brightness GaN-based LED...Stimulated emission and lasing of GaN-based laser diodes(LDs)were reported at 1995[1]and 1996[2],right after the breakthrough of p-type doping[3−5],material quality[6]and the invention of high-brightness GaN-based LEDs[7,8].However,it took much longer time for GaN-based LDs to achieve high power,high wall plug efficiency,and long lifetime.Until 2019,Nichia reported blue LDs with these performances[9],which open wide applications with GaN-based blue LDs.展开更多
To fully exploit the superiority of tubular structures,in this study,we systematically explore the optimal preparation conditions for Ni/Co_(3)O_(4),including cation species and content,additive species and content,an...To fully exploit the superiority of tubular structures,in this study,we systematically explore the optimal preparation conditions for Ni/Co_(3)O_(4),including cation species and content,additive species and content,and anion species.Our results reveal that the formation of an initial cobalt nickel acetate hydroxide prism is the key factor and directly affects the final microtubular structure.Moreover,P is subsequently doped into the Ni/Co_(3)O_(4)lattice to increase the M^(3+)/M^(2+)molar ratio(M=Co and Ni),promote reaction kinetics,and optimize electronic structure.Consequently,the oxygen evolution reaction performance of P-doped tubular Ni/Co_(3)O_(4)is significantly higher than that of undoped Ni/Co_(3)O_(4)and the state-of-the-art RuO_(2)electrocatalyst.展开更多
Application of transition metal boride(TMB) catalysts towards hydrolysis of NaBH_(4) holds great significance to help relieve the energy crisis. Herein, we present a facile and versatile metal-organic framework(MOF) a...Application of transition metal boride(TMB) catalysts towards hydrolysis of NaBH_(4) holds great significance to help relieve the energy crisis. Herein, we present a facile and versatile metal-organic framework(MOF) assisted strategy to prepare Co_(2)B-CoPO_x with massive boron vacancies by introducing phytic acid(PA) cross-linked Co complexes that are acquired from reaction of PA and ZIF-67 into cobalt boride. The PA etching effectively breaks down the structure of ZIF-67 to create more vacancies, favoring the maximal exposure of active sites and elevation of catalytic activity. Experimental results demonstrate a drastic electronic interaction between Co and the dopant phosphorous(P), thereby the robustly electronegative P induces electron redistribution around the metal species, which facilitates the dissociation of B-H bond and the adsorption of H_(2)O molecules. The vacancy-rich Co_(2)B-CoPO_x catalyst exhibits scalable performance, characterized by a high hydrogen generation rate(HGR) of 7716.7 m L min^(-1)g^(-1) and a low activation energy(Ea) of 44.9 k J/mol, rivaling state-of-the-art catalysts. This work provides valuable insights for the development of advanced catalysts through P doping and boron vacancy engineering and the design of efficient and sustainable energy conversion systems.展开更多
TiO2 films have received increasing attention for the removal of organic pollutants via photocatalysis. To develop a simple and effective method for improving the photodegradation efficiency of pollutants in surface w...TiO2 films have received increasing attention for the removal of organic pollutants via photocatalysis. To develop a simple and effective method for improving the photodegradation efficiency of pollutants in surface water, we herein examined the preparation of a P25-TiO2 composite film on a cement substrate via a sol–gel method. In this case, Rhodamine B（Rh B）was employed as the target organic pollutant. The self-generated TiO2 film and the P25-TiO2 composite film were characterized by X-ray diffraction（XRD）, N2 adsorption/desorption measurements, scanning electron microscopy（SEM）, transmission electron microscopy（TEM）, and diffuse reflectance spectroscopy（DRS）. The photodegradation efficiencies of the two films were studied by Rh B removal in water under UV（ultraviolet） irradiation. Over 4 day exposure, the P25-TiO2 composite film exhibited higher photocatalytic performance than the self-generated TiO2 film. The photodegradation rate indicated that the efficiency of the P25-TiO2 composite film was enhanced by the addition of the rutile phase Degussa P25 powder. As such, cooperation between the anatase TiO2 and rutile P25 nanoparticles was beneficial for separation of the photo-induced electrons and holes. In addition, the influence of P25 doping on the P25-TiO2 composite films was evaluated. We found that up to a certain saturation point, increased doping enhanced the photodegradation ability of the composite film. Thus, we herein demonstrated that the doping of P25 powders is a simple but effective strategy to prepare a P25-TiO2 composite film on a cement substrate, and the resulting film exhibits excellent removal efficiency in the degradation of organic pollutants.展开更多
The present paper is about a contribution to the bifacial PV cell performances improvement. The PV cell efficiency is weak compared to the strong energy demand. In this study, the base thickness impacts and the p+<...The present paper is about a contribution to the bifacial PV cell performances improvement. The PV cell efficiency is weak compared to the strong energy demand. In this study, the base thickness impacts and the p+</sup> zone size influence are evaluated on the rear face of the polycrystalline back surface field bifacial silicon PV cell. The photocurrent density and photovoltage behaviors versus thickness of these regions are studied. From a three-dimensional grain of the polycrystalline bifacial PV cell, the magneto-transport and continuity equations of excess minority carriers are solved to find the expression of the density of excess minority carriers and the related electrical parameters, such as the photocurrent density, the photovoltage and the electric power for simultaneous illumination on both sides. The photocurrent density, the photovoltage and electric power versus junction dynamic velocity decrease for different thicknesses of base and the p+</sup> region increases for simultaneous illumination on both sides. It is found that the thickness of the p+</sup> region at 0.1 μm and the base size at 100 μm allow reaching the best bifacial PV cell performances. Consequently, it is imperative to consider the reduction in the thickness of the bifacial PV cell for exhibition of better performance. This reduced the costs and increase production speed while increasing conversion efficiency.展开更多
The reactivation and subsequent reuse of exhausted selective catalytic reduction(SCR)catalysts has significant economic and environmental advantages.Water and acid washing along with thermal regeneration are commonly ...The reactivation and subsequent reuse of exhausted selective catalytic reduction(SCR)catalysts has significant economic and environmental advantages.Water and acid washing along with thermal regeneration are commonly used to eliminate toxic substances from the catalyst surface,while these processes often result in the undesired loss of active components.In this research,an impregnation approach was adopted to replenish the depleted active constituents of the spent V_(2)O_(5)-WO_(3)/TiO_(2)(VW/Ti)catalyst.Experimental investigations were conducted to evaluate the influence of Ce/P doping on both the SCR activity of this rejuvenated catalyst and its resistance to the detrimental effects of SO_(2)/H_(2)O exposure.The optimal performance is achieved with the Ce/P co-doped VW/Ti catalyst,demonstrating remarkable efficiency in removing nearly 100%of NO_(x)across a broad range of temperatures from 150 to 450℃.The incorporation of a proper content of Ce serves to increase the VOx surface density from a sub-monolayer state to a monolayer state and fosters the formation of more surface oxygen vacancies.This transformation positively contributes to enhancing both the catalytic activity and the resistance to SO_(2)/H_(2)O poisoning.Further treatment with H3PO4,although rendering the catalyst more susceptible to H_(2)O,achieves a delicate balance between its surface acidity and redox capabilities.This optimized state not only enhances the catalyst's robustness but also further widens the active temperature window.展开更多
Surface engineering has been found to be an efficient strategy to boost the catalytic performance of noble-metal-based nanocatalysts.In this work,a small amount of P was doped to the surface of PtNi concave cube(P-PtN...Surface engineering has been found to be an efficient strategy to boost the catalytic performance of noble-metal-based nanocatalysts.In this work,a small amount of P was doped to the surface of PtNi concave cube(P-PtNi CNC).Interestingly,the P-PtNi CNC nanocatalyst shows an enhanced methanol oxidation reaction(MOR)performance with achieving 8.19 times of specific activity than that of comercial Pt/C.The electrochemical in situ Fourier transform infrared spectroscopy(FTIR)results reveal that the surface P doping promotes the adsorption energy of OH,enhancing the resistance against CO poisoning.Therefore,the intermediate adsorbed CO(COads)reacted with adsorbed OH(OHads)through the Langmuir–Hinshelwood(LH)mechanism to generate CO_(2)and release surface active sites for further adsorption.This work provides a promising strategy via the incorporation of non-metallic elements into the PtNi alloys bounded with high-index facets(HIFs)as efficient fuel cell catalysts.展开更多
The non-noble Mn coordinated N,P co-doping graphene materials were investigated theoretically in this work based on density functional theory calculation.The electronic structure is effectively tuned after the introdu...The non-noble Mn coordinated N,P co-doping graphene materials were investigated theoretically in this work based on density functional theory calculation.The electronic structure is effectively tuned after the introduction of P heteroatom.The moderate d band center and density of states at Fermi energy of MnN_(4)-P1-G indicate that it is ofmodest adsorption ability for these O-containing intermediates.The rank of adsorption energies ofO-containing intermediates for MnN_(4)-P1-G is OH*>2OH*>OOH*>O*>O2*>H2O*,whereas the MnN_(4)-P1-G favors a four-electron process instead of two-electron process.The doping of P on MnN_(4)-P1-G can increase the kinetic activity for the rate-determining step as well as the Ulim for MnN_(4)-P1-G significantly increases from 0.38 to 0.45 V compared with MnN_(4)-G.The spin density and magnetic moments of Mn are effectively tuned by d,p hybridization to lower the adsorption energy ofOHintermediates(rate-determining step[RDS])so as to improve the catalytic activity.It is concluded that the P-doped MnN_(4)catalysts with excellent oxygen reduction reaction activity can be obtained and this study can provide theoretical guidance for the rational design of high-performanceMn-based carbonmaterials catalysts.展开更多
Sodium ion hybrid capacitors(SIHCs)are regarded as advanced power supply systems.Nevertheless,the kinetics imbalance of cathode and anode suppresses the further performance improvement of SIHCs.The carbonaceous anode ...Sodium ion hybrid capacitors(SIHCs)are regarded as advanced power supply systems.Nevertheless,the kinetics imbalance of cathode and anode suppresses the further performance improvement of SIHCs.The carbonaceous anode materials are promising and many strategies have been utilized to increase the capacity of sloping region or accelerate the reaction rate of plateau region.However,it is still challenging to simultaneously realize high mesopore/micropore volume ratio,large interlayer distance(>0.37 nm),and abundant and favorable heteroatoms-doping by a simple method.Herein,we report N,P,O ternarydoped mesoporous carbon(PNPOC-T,T=700,800 or 900)with large interlayer distance(~0.4 nm)as anode materials.The PNPOC-T were prepared by a simple in-situ polymerization of aniline and phytic acid on the exfoliated graphitic nitrogen carbide(g-C3N4)and subsequent carbonization.The obtained PNPOC-800 exhibits an excellent rate performance(101.5 mA·h·g^(-1) at 20 A·g^(-1)),which can be attributed to the high surface-controlled capacitive behavior ratio and rapid ion diffusion.The optimum SIHCs display a high energy density of 105.48 W·h·kg^(-1) and a high power density of 13.59 kW$kg1.Furthermore,the capacitance retention rate of SIHCs can reach 87.43%after 9000 cycles at 1 A·g^(-1).展开更多
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.22178148 and 22278193)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘As a catalyst of the air cathode in zinc-air batteries,tungstic acid ferrous(FeWO_(4)),a nanoscale transition metal tungstate,shows a broad application prospect in the oxygen reduction reaction(ORR).While FeWO_(4)possesses favorable electrochemical properties and thermodynamic stability,its intrinsic semiconductor characteristics result in a relatively slow electron transfer rate,limiting the ORR catalytic activity.In this work,the electronic structure of FeWO_(4)is significantly modulated by introducing phosphorus(P)atoms with abundant valence electrons.The P doping can adjust the electronic structure of FeWO_(4)and then optimize oxygen-containing intermediates'absorption/desorption efficiency to achieve improved ORR activity.Furthermore,the sodium chloride template is utilized to construct a porous carbon framework for anchoring phosphorus-doped iron tungstate(P-FeWO_(4)/PNC).The porous carbon skeleton provides numerous active sites for the absorption/desorption and redox reactions on the P-FeWO_(4)/PNC surface and serves as mass transport channels for reactants and intermediates.The P-FeWO_(4)/PNC demonstrates ORR performance(E1/2=0.86 V vs.RHE).Furthermore,the zinc-air batteries incorporating the P-FeWO_(4)/PNC composite demonstrate an increased peak power density(172.2 mW·cm^(-2)),high specific capacity(810.1 mAh·g^(-1)),and sustained long-term cycling stability lasting up to 240 h.This research not only contributes to the advancement of cost-effective tungsten-based non-precious metallic ORR catalysts,but also guides their utilization in zinc-air batteries.
基金financially supported by the National Natural Science Foundation of China(52472248 and 22075221)the Key Research and Development Project of Shanxi Province(202202060301003 and 202202060301015)the Innovation Program of Wuhan-Shuguang Project(2023010201020367)。
文摘Poly(3-hexylthiophene)(P3HT)is one of the most promising hole-transporting materials in the pursuit of efficient and stable perovskite solar cells due to its outstanding stability and low cost.However,the intrinsic low carrier density of P3 HT and poor contact between the P3HT/perovskite interface always lead to a low performance of the solar cell,while conventional chemical doping always makes the films unstable and limits the scalability.In this work,for the first time,we simultaneously enhanced the hole transporting properties of P3HT film and the interface of perovskite by doping it with a judiciously designed oxidized small molecule organic semiconductor.The organic salt not only can promote the lamellar crystallinity of P3HT to obtain better charge transport properties,but also reduce the defects of perovskite.As a result,we achieved champion efficiencies of 23.0%for small-area solar cells and 18.8%for larger-area modules(48.0 cm^(2)).This efficiency is the highest value for P3HT-based perovskite modules.Moreover,the solar cells show excellent operational stability,retaining over 95%of their initial efficiencies after1200 h of continuous operation.
基金supported by Zhejiang Provincial Natural Science Foundation of China(No.LTGS23B030002)the National Natural Science Foundation of China(Nos.21978111 and 22278175)。
文摘Traditional photo-electcatalyst structures of small noble metal nanoparticles assembling into large-scale photoactive semiconductors still suffer from agglomeration of noble metal nanoparticles,insufficient charge transfer,undesirable photoresponse ability that restricted the photo-electrocatalytic performance.To this end,a novel design strategy is proposed in this work,namely integrating small-scale photoactive materials(doped graphene quantum dots,S,N-GQDs)with large-sized noble metal(Pd P)nanoflowers to form novel photo-electrocatalysts for high-efficient alcohol oxidation reaction.As expected,superior electrocatalytic performance of Pd P/S,N-GQDs for ethylene glycol oxidation is acquired,thanks to the nanoflower structure with larger specific surface area and abundant active sites.Furthermore,nonmetal P are demonstrated,especially optimizing the adsorption strength,enhancing the interfacial contact,reducing metal agglomeration,ensuring uniform and efficient doping of S,N-GQDs,and ultimately significantly boost the catalytic activity of photo-electrocatalysts.
基金supported by the Natural Science Foundation of Jiangsu Province(Grant.BK20232042).
文摘Stimulated emission and lasing of GaN-based laser diodes(LDs)were reported at 1995[1]and 1996[2],right after the breakthrough of p-type doping[3−5],material quality[6]and the invention of high-brightness GaN-based LEDs[7,8].However,it took much longer time for GaN-based LDs to achieve high power,high wall plug efficiency,and long lifetime.Until 2019,Nichia reported blue LDs with these performances[9],which open wide applications with GaN-based blue LDs.
文摘To fully exploit the superiority of tubular structures,in this study,we systematically explore the optimal preparation conditions for Ni/Co_(3)O_(4),including cation species and content,additive species and content,and anion species.Our results reveal that the formation of an initial cobalt nickel acetate hydroxide prism is the key factor and directly affects the final microtubular structure.Moreover,P is subsequently doped into the Ni/Co_(3)O_(4)lattice to increase the M^(3+)/M^(2+)molar ratio(M=Co and Ni),promote reaction kinetics,and optimize electronic structure.Consequently,the oxygen evolution reaction performance of P-doped tubular Ni/Co_(3)O_(4)is significantly higher than that of undoped Ni/Co_(3)O_(4)and the state-of-the-art RuO_(2)electrocatalyst.
基金supported by the National Natural Science Foundation of China (No.21965005)Natural Science Foundation of Guangxi Province (No.2021GXNSFAA076001)+1 种基金Guangxi Technology Base and Talent Subject (Nos.GUIKE AD18126001, GUIKE AD20297039)Innovation Project of Guangxi Graduate Education (Nos.YCSW2023140, YCBZ2023062)。
文摘Application of transition metal boride(TMB) catalysts towards hydrolysis of NaBH_(4) holds great significance to help relieve the energy crisis. Herein, we present a facile and versatile metal-organic framework(MOF) assisted strategy to prepare Co_(2)B-CoPO_x with massive boron vacancies by introducing phytic acid(PA) cross-linked Co complexes that are acquired from reaction of PA and ZIF-67 into cobalt boride. The PA etching effectively breaks down the structure of ZIF-67 to create more vacancies, favoring the maximal exposure of active sites and elevation of catalytic activity. Experimental results demonstrate a drastic electronic interaction between Co and the dopant phosphorous(P), thereby the robustly electronegative P induces electron redistribution around the metal species, which facilitates the dissociation of B-H bond and the adsorption of H_(2)O molecules. The vacancy-rich Co_(2)B-CoPO_x catalyst exhibits scalable performance, characterized by a high hydrogen generation rate(HGR) of 7716.7 m L min^(-1)g^(-1) and a low activation energy(Ea) of 44.9 k J/mol, rivaling state-of-the-art catalysts. This work provides valuable insights for the development of advanced catalysts through P doping and boron vacancy engineering and the design of efficient and sustainable energy conversion systems.
基金supported by the National Science Funds for Creative Research Groups of China (No. 51421006)the National Major Projects of Water Pollution Control and Management Technology (No. 2017ZX07204003)+2 种基金the National Key Plan for Research and Development of China (2016YFC0502203)the Key Program of National Natural Science Foundation of China (No. 91647206)the Qing Lan Project of Jiangsu Province, and PAPD
文摘TiO2 films have received increasing attention for the removal of organic pollutants via photocatalysis. To develop a simple and effective method for improving the photodegradation efficiency of pollutants in surface water, we herein examined the preparation of a P25-TiO2 composite film on a cement substrate via a sol–gel method. In this case, Rhodamine B（Rh B）was employed as the target organic pollutant. The self-generated TiO2 film and the P25-TiO2 composite film were characterized by X-ray diffraction（XRD）, N2 adsorption/desorption measurements, scanning electron microscopy（SEM）, transmission electron microscopy（TEM）, and diffuse reflectance spectroscopy（DRS）. The photodegradation efficiencies of the two films were studied by Rh B removal in water under UV（ultraviolet） irradiation. Over 4 day exposure, the P25-TiO2 composite film exhibited higher photocatalytic performance than the self-generated TiO2 film. The photodegradation rate indicated that the efficiency of the P25-TiO2 composite film was enhanced by the addition of the rutile phase Degussa P25 powder. As such, cooperation between the anatase TiO2 and rutile P25 nanoparticles was beneficial for separation of the photo-induced electrons and holes. In addition, the influence of P25 doping on the P25-TiO2 composite films was evaluated. We found that up to a certain saturation point, increased doping enhanced the photodegradation ability of the composite film. Thus, we herein demonstrated that the doping of P25 powders is a simple but effective strategy to prepare a P25-TiO2 composite film on a cement substrate, and the resulting film exhibits excellent removal efficiency in the degradation of organic pollutants.
文摘The present paper is about a contribution to the bifacial PV cell performances improvement. The PV cell efficiency is weak compared to the strong energy demand. In this study, the base thickness impacts and the p+</sup> zone size influence are evaluated on the rear face of the polycrystalline back surface field bifacial silicon PV cell. The photocurrent density and photovoltage behaviors versus thickness of these regions are studied. From a three-dimensional grain of the polycrystalline bifacial PV cell, the magneto-transport and continuity equations of excess minority carriers are solved to find the expression of the density of excess minority carriers and the related electrical parameters, such as the photocurrent density, the photovoltage and the electric power for simultaneous illumination on both sides. The photocurrent density, the photovoltage and electric power versus junction dynamic velocity decrease for different thicknesses of base and the p+</sup> region increases for simultaneous illumination on both sides. It is found that the thickness of the p+</sup> region at 0.1 μm and the base size at 100 μm allow reaching the best bifacial PV cell performances. Consequently, it is imperative to consider the reduction in the thickness of the bifacial PV cell for exhibition of better performance. This reduced the costs and increase production speed while increasing conversion efficiency.
基金funded by the Shanghai Committee of Science and Technology(No.23010503500).
文摘The reactivation and subsequent reuse of exhausted selective catalytic reduction(SCR)catalysts has significant economic and environmental advantages.Water and acid washing along with thermal regeneration are commonly used to eliminate toxic substances from the catalyst surface,while these processes often result in the undesired loss of active components.In this research,an impregnation approach was adopted to replenish the depleted active constituents of the spent V_(2)O_(5)-WO_(3)/TiO_(2)(VW/Ti)catalyst.Experimental investigations were conducted to evaluate the influence of Ce/P doping on both the SCR activity of this rejuvenated catalyst and its resistance to the detrimental effects of SO_(2)/H_(2)O exposure.The optimal performance is achieved with the Ce/P co-doped VW/Ti catalyst,demonstrating remarkable efficiency in removing nearly 100%of NO_(x)across a broad range of temperatures from 150 to 450℃.The incorporation of a proper content of Ce serves to increase the VOx surface density from a sub-monolayer state to a monolayer state and fosters the formation of more surface oxygen vacancies.This transformation positively contributes to enhancing both the catalytic activity and the resistance to SO_(2)/H_(2)O poisoning.Further treatment with H3PO4,although rendering the catalyst more susceptible to H_(2)O,achieves a delicate balance between its surface acidity and redox capabilities.This optimized state not only enhances the catalyst's robustness but also further widens the active temperature window.
基金the National Natural Science Foundation of China(No.21573286)the Natural Science Foundation of Hebei Province of China(No.E2020408004)the Funded by Science and Technology Project of Hebei Education Department(No.QN2021124).
文摘Surface engineering has been found to be an efficient strategy to boost the catalytic performance of noble-metal-based nanocatalysts.In this work,a small amount of P was doped to the surface of PtNi concave cube(P-PtNi CNC).Interestingly,the P-PtNi CNC nanocatalyst shows an enhanced methanol oxidation reaction(MOR)performance with achieving 8.19 times of specific activity than that of comercial Pt/C.The electrochemical in situ Fourier transform infrared spectroscopy(FTIR)results reveal that the surface P doping promotes the adsorption energy of OH,enhancing the resistance against CO poisoning.Therefore,the intermediate adsorbed CO(COads)reacted with adsorbed OH(OHads)through the Langmuir–Hinshelwood(LH)mechanism to generate CO_(2)and release surface active sites for further adsorption.This work provides a promising strategy via the incorporation of non-metallic elements into the PtNi alloys bounded with high-index facets(HIFs)as efficient fuel cell catalysts.
基金State Key Laboratory of UrbanWater Resource and Environment,Harbin Institute of Technology,China,Grant/Award Number:2021TS07。
文摘The non-noble Mn coordinated N,P co-doping graphene materials were investigated theoretically in this work based on density functional theory calculation.The electronic structure is effectively tuned after the introduction of P heteroatom.The moderate d band center and density of states at Fermi energy of MnN_(4)-P1-G indicate that it is ofmodest adsorption ability for these O-containing intermediates.The rank of adsorption energies ofO-containing intermediates for MnN_(4)-P1-G is OH*>2OH*>OOH*>O*>O2*>H2O*,whereas the MnN_(4)-P1-G favors a four-electron process instead of two-electron process.The doping of P on MnN_(4)-P1-G can increase the kinetic activity for the rate-determining step as well as the Ulim for MnN_(4)-P1-G significantly increases from 0.38 to 0.45 V compared with MnN_(4)-G.The spin density and magnetic moments of Mn are effectively tuned by d,p hybridization to lower the adsorption energy ofOHintermediates(rate-determining step[RDS])so as to improve the catalytic activity.It is concluded that the P-doped MnN_(4)catalysts with excellent oxygen reduction reaction activity can be obtained and this study can provide theoretical guidance for the rational design of high-performanceMn-based carbonmaterials catalysts.
基金supported by the National Nature Science Foundation of China(Nos.52172047,51972191)and the National Key Research and Development Program of China(No.2021YFA1200800).
文摘Sodium ion hybrid capacitors(SIHCs)are regarded as advanced power supply systems.Nevertheless,the kinetics imbalance of cathode and anode suppresses the further performance improvement of SIHCs.The carbonaceous anode materials are promising and many strategies have been utilized to increase the capacity of sloping region or accelerate the reaction rate of plateau region.However,it is still challenging to simultaneously realize high mesopore/micropore volume ratio,large interlayer distance(>0.37 nm),and abundant and favorable heteroatoms-doping by a simple method.Herein,we report N,P,O ternarydoped mesoporous carbon(PNPOC-T,T=700,800 or 900)with large interlayer distance(~0.4 nm)as anode materials.The PNPOC-T were prepared by a simple in-situ polymerization of aniline and phytic acid on the exfoliated graphitic nitrogen carbide(g-C3N4)and subsequent carbonization.The obtained PNPOC-800 exhibits an excellent rate performance(101.5 mA·h·g^(-1) at 20 A·g^(-1)),which can be attributed to the high surface-controlled capacitive behavior ratio and rapid ion diffusion.The optimum SIHCs display a high energy density of 105.48 W·h·kg^(-1) and a high power density of 13.59 kW$kg1.Furthermore,the capacitance retention rate of SIHCs can reach 87.43%after 9000 cycles at 1 A·g^(-1).
