The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-...The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.展开更多
To effectively address energy challenges,it is crucial to explore efficient and stable bifunctional nonprecious metal catalysts.In this study,a Mo-doped nickeliron layered double hydroxide with flower-cluster architec...To effectively address energy challenges,it is crucial to explore efficient and stable bifunctional nonprecious metal catalysts.In this study,a Mo-doped nickeliron layered double hydroxide with flower-cluster architecture was successfully prepared by a one-step hydrothermal method,which demonstrated a good water splitting performance.After an appropriate amount of Mo doping,some lattice distortions in the material provided reactive sites for the adsorption and conversion of intermediates,thus optimising the charge distribution of the material.Moreover,the multidimensional void structures formed after doping had a larger specific surface area and accelerated the penetration of the electrolyte,which significantly improved the activity of the catalyst in alkaline media.At 10 mA·cm^(-2),the hydrogen and oxygen evolution overpotentials of Mo-doped nickel-iron double hydroxides(Mo-NiFe LDH/NF-0.2)were 167 and 220 mV,respectively,with an excellent durability up to 24 h.When the Mo-NiFe LDH/NF-0,2 catalyst was used as the cathode and anode of an electrolytic cell,the catalyst achieved a current density of 10 mA·cm^(-2)at an applied voltage of 1.643 V.This study provides a novel approach for designing excellent bifunctional electrocatalysts containing nonprecious metals.展开更多
Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic ch...Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic chlorine.Especially,it is full of challenges to unveil the key factors influencing the selectivity of such complex PEC processes.Herein,by regulating the energy band and surface structure of the anatase TiO_(2) nanotube array photoanode via nitrogen-doping,the seawater PEC oxidation shifts from Cl^(-)oxidation reaction(ClOR)dominant on the TiO_(2) photoanode(61.6%)to oxygen evolution reaction(OER)dominant on the N-TiO_(2) photoanode(62.9%).Comprehensive investigations including operando photoelectrochemical FTIR and DFT calculations unveil that the asymmetric hydrogen-bonding water at the N-TiO_(2) electrode/electrolyte interface enriches under illumination,facilitating proton transfer and moderate adsorption strength of oxygen-intermediates,which lowers the energy barrier for the OER yet elevates the energy barrier for the ClOR,resulting to a promoted selectivity towards the OER.The work sheds light on the underlying mechanism of the PEC water oxidation processes,and highlights the crucial role of interfacial water on the PEC selectivity,which could be regulated by controlling the energy band and the surface structure of semiconductors.展开更多
Altermagnets represent a newly discovered class of magnetically ordered materials.Among all the candidates,CrSb stands out due to its largest spin splitting energy and highest Néel temperature exceeding 700 K,mak...Altermagnets represent a newly discovered class of magnetically ordered materials.Among all the candidates,CrSb stands out due to its largest spin splitting energy and highest Néel temperature exceeding 700 K,making it promising for room-temperature spintronic applications.Here we have successfully grown high quality CrSb(100)thin film on GaAs(110)substrate by molecular beam epitaxy.Using angle-resolved photoemission spectroscopy,we successfully obtained the three-dimensional electronic structure of the thin film.Moreover,we observed the emergence of the altermagnetic splitting bands corresponding to the calculated results along the low symmetry pathsT-QandP-D.The bands near the Fermi level are only spin splitting bands along theP-Ddirection,with splitting energy reaching as high as 910 meV.This finding provides insights into the magnetic properties of CrSb thin films and paves the way for further studies on their electronic structure and potential applications in spintronics.展开更多
This study investigates the dynamic compressive behavior of three periodic lattice structures fabricated from Ti-6Al-4V titanium alloy,each with distinct topologies:simple cubic(SC),body-centered cubic(BCC),and face-c...This study investigates the dynamic compressive behavior of three periodic lattice structures fabricated from Ti-6Al-4V titanium alloy,each with distinct topologies:simple cubic(SC),body-centered cubic(BCC),and face-centered cubic(FCC).Dynamic compression experiments were conducted using a Split Hopkinson Pressure Bar(SHPB)system,complemented by high-speed imaging to capture real-time deformation and failure mechanisms under impact loading.The influence of cell topology,relative density,and strain rate on dynamic mechanical properties,failure behavior,and stress wave propagation was systematically examined.Finite element modeling was performed,and the simulated results showed good agreement with experimental data.The findings reveal that the dynamic mechanical properties of the lattice structures are generally insensitive to strain rate variations,while failure behavior is predominantly governed by structural configuration.The SC structure exhibited strut buckling and instability-induced fracture,whereas the BCC and FCC structures displayed layer-by-layer crushing with lower strain rate sensitivity.Regarding stress wave propagation,all structures demonstrated significant attenuation capabilities,with the BCC structure achieving the greatest reduction in transmitted wave amplitude and energy.Across all configurations,wave reflection was identified as the primary energy dissipation mechanism.These results provide critical insights into the design of lattice structures for impact mitigation and energy absorption applications.展开更多
This study,a core-shell CoPt@C assembled hierarchical catalyst(named CoPt@C)was prepared using a unique CH_(4)deposition strategy for highly efficient overall water splitting.CoPt@C is composed of dense CoPt@C core-sh...This study,a core-shell CoPt@C assembled hierarchical catalyst(named CoPt@C)was prepared using a unique CH_(4)deposition strategy for highly efficient overall water splitting.CoPt@C is composed of dense CoPt@C core-shell nanoparticles(NPs)and a minor proportion of curled CoPt@nanotubes(CoPt@CNTs).Moreover,by adjusting the CH_(4)deposition time,the carbon shell thickness can be effectively regulated.Benefiting from the synergistic interaction between CoPt alloy and carbon shell,coupled with the high conductivity of the carbon shell,the overpotential of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)for CoPt@C is 15 and 120 mV at 10 mA cm^(-2).In addition,CoPt@C requires only 1.58 V to achieve 10 mA cm^(-2)for overall water splitting and maintains excellent stability over 80 h of continuous electrolysis.Density functional theory(DFT)calculations suggest that electrons transfer from the CoPt alloy NPs to the carbon shell,rendering the carbon shell electron-rich.Additionally,the hydrogen adsorption energy(ΔG*H)and the rate-determining step(ΔG*OOH)on CoPt@C are only-0.22 and 1.9 eV,respectively.展开更多
Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxy...Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this work,we synthesized a self-supporting heterogeneous NiSe@Co_(0.85)Se/NF electrocatalyst using a facile in situ selenization of transition metal precursors that coated on the nickel foam(NF)in polyol solution.The NF was used as both conductive substrate and nickel source,ensuring superior electronic conductivity for catalyzing.The NiSe@-Co_(0.85)Se/NF exhibited remarkable bifunctional electrocatalytic activities with HER overpotential of 168 mV and OER overpotential of 258 mV to achieve 10 mA·cm-2.The water splitting system using NiSe@Co_(0.85)Se/NF as both anode and cathode electrodes achieved a current density of 10 mA·cm^(-2) at 1.61 V with nearly 100% faradaic efficiency and impressively long-term stability.The efficient bifunctional catalytic performance of NiSe@-Co_(0.85)Se/NF should be attributed to the electronic modulation and synergistic effect between NiSe and Co_(0.85)Se,the intrinsic metallic conductivity and the enlarged active sites exposure.This work provides a facile method for developing heterogeneous bifunctional catalysts for advanced electrochemical energy conversion technologies.展开更多
Stable non-noble metal bifunctional electrocatalysts are one of the challenges to the fluctuating overall water splitting driven by re-newable energy.Herein,a novel self-supporting hierarchically porous Ni_(x)Fe-S/NiF...Stable non-noble metal bifunctional electrocatalysts are one of the challenges to the fluctuating overall water splitting driven by re-newable energy.Herein,a novel self-supporting hierarchically porous Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure as bifunctional electrocatalyst was constructed based on porous Ni-Fe electrodeposition on three-dimensional(3D)carbon fiber cloth,in situ oxidation,and chemical sulfuration.Results showed that the Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure with a large specific surface area exhibits good bifunctional activity and stability for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)because of the abundance of active sites,synergistic effect of the heterostructure,superhydrophilic surface,and stable,self-supporting structure.The results further confirmed that the Ni_(x)Fe-S phase in the heterostructure is transformed into metal oxides/hydroxides and Ni_(3)S_(2) during OER.Compared with the commercial 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer,the self-supporting Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) electrolyzer exhibits better stability and lower cell voltage in the fluctu-ating current density range of 10-500 mA/cm^(2).Particularly,the cell voltage of Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) is only approximately 3.91 V at an industrial current density of 500 mA/cm^(2),which is lower than that of the 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer(i.e.,approximately 4.79 V).This work provides a promising strategy to develop excellent bifunctional electrocatalysts for fluctuating overall water splitting.展开更多
Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of...Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of TMPs.Herein,a novel method for synthesizing CoP nanoparticles encapsu-lated in a rich-defect carbon shell(CoP/DCS)is developed through the self-assembly of modified polycyclic aromatic molecules.The graft and removal of high-activity C-N bonds of aromatic molecules render the controllable design of crystallite defects of carbon shell.The density functional theory calculation indicates that the carbon defects with unpaired electrons could effectively tailor the band structure of CoP.Benefiting from the improved activity and corrosion resistance,the CoP/DCS delivers outstanding difunctional hydrogen evolution reaction(88 mV)and oxygen evolution reaction(251 mV)performances at 10 mA cm^(−2)current density.Furthermore,the coupled water electrolyzer with CoP/DCS as both the cathode and anode presents ultralow cell voltages of 1.49 V to achieve 10 mA cm^(−2)with long-time stability.This strategy to improve TMPs electrocatalyst with rich-DCS and heterogeneous structure will inspire the design of other transition metal compound electrocatalysts for water splitting.展开更多
Photoelectrochemical(PEC) water splitting offers the capability of harvesting, storing, and converting solar energy into clean and sustainable hydrogen energy. Metal oxides are appealing photoelectrode materials becau...Photoelectrochemical(PEC) water splitting offers the capability of harvesting, storing, and converting solar energy into clean and sustainable hydrogen energy. Metal oxides are appealing photoelectrode materials because of their easy manufacturing and relatively high stability. In particular, metal oxides prepared by electrochemical anodization are typical of ordered nanostructures, which are beneficial for light harvesting, charge transfer and transport, and the adsorption and desorption of reactive species due to their high specific surface area and rich channels. However, bare anodic oxides still suffer from low charge separation and sunlight absorption efficiencies. Accordingly, many strategies of modifying anodic oxides have been explored and investigated. In this review, we attempt to summarize the recent advances in the rational design and modifications of these oxides from processes before, during, and after anodization. Rational design strategies are thoroughly addressed for each part with an aim to boost overall PEC performance. The ongoing efforts and challenges for future development of practical PEC electrodes are also presented.展开更多
A comprehensive theoretical study of correlation effects on the fine-structure splitting within the ground configuration 3d9 of the Co-like HI45＋, Ta46＋, W47＋, and Au52＋ ions is performed by employing the multi-co...A comprehensive theoretical study of correlation effects on the fine-structure splitting within the ground configuration 3d9 of the Co-like HI45＋, Ta46＋, W47＋, and Au52＋ ions is performed by employing the multi-configuration Dirac-Hartree- Fock method in the active space approximation. It shows that the core-valence correlation with the inner-core 2p electron is more significant than with the outer 3p and 3s electrons, and the correlation with the 2s electron is also noticeable. The core-core correlation seems to be small and can be ignored. The calculated 2D3/2,5/2 splitting energies agree with the recent electron-beam ion-trap measurements [Phys. Rev. A 83 032517 （2011）, Eur. Phys. J. D 66 286 （2012）] to within the experimental uncertainties.展开更多
The inter-relation between zero-field splitting （ZFS） parameters and local lattice structures of the （CrSe4）6 clusters in ZnSe semiconductors has been established by using the complete diagonalization （of the ene...The inter-relation between zero-field splitting （ZFS） parameters and local lattice structures of the （CrSe4）6 clusters in ZnSe semiconductors has been established by using the complete diagonalization （of the energy matrix） method. On the basis of this, the local lattice distortions, the ZFS parameters D, a, F and the optical spectrum for Cr2＋ ions doped into ZnSe are theoretically investigated, and the contributions of the spin singlets have been taken into account. The calculated ZFS parameters are in good agreement with the experimental values. From our calculations, the tetragonal distortion parameters AR = 0.091A and Aθ = 4.28° of Cr2＋ in ZnSe are acquired, and the results suggest that there exists a tetragonal expansion distortion for the local lattice structure of （CrSe4）6- clusters in ZnSe crystals. The influence of the spin singlets on ZFS parameters is also discussed, indicating that the contributions to ZFS parameters a and F cannot be ignored.展开更多
Designing and synthesizing cost-effective bifunctional catalysts for overall alkaline water/seawater splitting is still a huge challenge for hydrogen production.Herein,Co/Ni/Fe/Mn based-amorphous high-entropy phosphox...Designing and synthesizing cost-effective bifunctional catalysts for overall alkaline water/seawater splitting is still a huge challenge for hydrogen production.Herein,Co/Ni/Fe/Mn based-amorphous high-entropy phosphoxide self-standing electrode(CNFMPO)is synthesized by the facile and fast electrodeposition method.CNFMPO exhibits excellent bifunctional electrocatalytic performances on alkaline water/seawater electrolysis.The hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)overpotentials of CNFMPO in alkaline water/seawater are as low as 43/73 and 252/282 mV to reach a current density of 10 mA cm^(-2),respectively.Additionally,two-electrode electrolyzers with CNFMPO||CNFMPO successfully achieve the current density of 10 mA cm^(-2) at low voltages of 1.54 and 1.56 V for overall alkaline water/seawater splitting,respectively.CNFMPO exhibits satisfactory long-term stability on overall alkaline water/seawater splitting for the surface reconstruction into active metal hydroxide/(oxy)hydroxide,phosphite,and phosphate.Moreover,no hypochlorite is detected during seawater electrolysis for the beneficial chlorite oxidation inhibition of the reconstructed phosphite and phosphate.The excellent catalytic performances of CNFMPO are due to the unique amorphous structure,multi-component synergistic effect,beneficial electronic structure modulation,and surface reconstruction during the catalytic reaction process.Therefore,CNFMPO has shown potential promotion to the development of the water/seawater splitting industry as a promising substituent for noble-metal electrocatalysts.This work provides new insights into the design of efficient bifunctional catalysts for overall water/seawater splitting.展开更多
Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of nove...Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and Au.The electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and HER.Impressively,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 V.Moreover,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was assembled.Accordingly,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS equipment.The interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.展开更多
Transition metal phosphides(TMPs)have emerged as an alternative to precious metals as efficient and low-cost catalysts for water electrolysis.Elemental doping and morphology control are effective approaches to further...Transition metal phosphides(TMPs)have emerged as an alternative to precious metals as efficient and low-cost catalysts for water electrolysis.Elemental doping and morphology control are effective approaches to further improve the performance of TMPs.Herein,Fe-doped CoP nanoframes(Fe-CoP NFs)with specific open cage configuration were designed and synthesized.The unique nano-framework structured Fe-CoP material shows overpotentials of only 255 and 122 mV at 10 mA cm^(−2)for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER),respectively,overwhelming most transition metal phosphides.For overall water splitting,the cell voltage is 1.65 V for Fe-CoP NFs at a current density of 10 mA cm^(−2),much superior to what is observed for the classical nanocubic structures.Fe-CoP NFs show no activity degradation up to 100 h which contrasts sharply with the rapidly decaying performance of noble metal catalyst reference.The superior electrocatalytic performance of Fe-CoP NFs due to abundant accessible active sites,reduced kinetic energy barrier,and preferable*O-containing intermediate adsorption is demonstrated through experimental observations and theoretical calculations.Our findings could provide a potential method for the preparation of multifunctional material with hollow structures and offer more hopeful prospects for obtaining efficient earth-abundant catalysts for water splitting.展开更多
DC-inverter split air-conditioner is widely used in Chinese homes as a result of its high-efficiency and energy-saving. Recently, the researches on its outdoor unit have focused on the influence of surrounding structu...DC-inverter split air-conditioner is widely used in Chinese homes as a result of its high-efficiency and energy-saving. Recently, the researches on its outdoor unit have focused on the influence of surrounding structures upon the aerodynamic and acoustic performance, however they are only limited to the influence of a few parameters on the performance, and practical design of the unit requires more detailed parametric analysis. Three-dimensional computational fluid dynamics（CFD） and computational aerodynamic acoustics（CAA） simulation based on FLUENT solver is used to study the influence of surrounding structures upon the aforementioned properties of the unit. The flow rate and sound pressure level are predicted for different rotating speed, and agree well with the experimental results. The parametric influence of three main surrounding structures（i.e. the heat sink, the bell-mouth type shroud and the outlet grille） upon the aerodynamic performance of the unit is analyzed thoroughly. The results demonstrate that the tip vortex plays a major role in the flow fields near the blade tip and has a great effect on the flow field of the unit. The inlet ring＇s size and throat＇s depth of the bell-mouth type shroud, and the through-flow area and configuration of upwind and downwind sections of the outlet grille are the most important factors that affect the aerodynamic performance of the unit. Furthermore, two improved schemes against the existing prototype of the unit are developed, which both can significantly increase the flow rate more than 6 %（i.e. 100 m3·h～（-1）） at given rotating speeds. The inevitable increase of flow noise level when flow rate is increased and the advantage of keeping a lower rotating speed are also discussed. The presented work could be a useful guideline in designing the aerodynamic and acoustic performance of the split air-conditioner in engineering practice.展开更多
The green hydrogen generation powered by renewable electricity promises the potential decarbonization of the hard-to-abate sector and is essential for the fulfillment of the Paris Agreement that attempts to limit the ...The green hydrogen generation powered by renewable electricity promises the potential decarbonization of the hard-to-abate sector and is essential for the fulfillment of the Paris Agreement that attempts to limit the global average temperature rise in the range of 1.5–2.0 ℃ above the pre-industrial level by the end of this century. Tremendous efforts have been devoted to the optimization of the electrocatalytic performance of the catalysts under industrial-relevant current densities via rational structure design,which induces a preferential electron distribution that favors the adsorption/desorption behavior of the key intermediates, thus accelerating the reaction kinetics. In this review, a brief introduction of the current energy status will be first presented to necessitate the importance of green hydrogen.Followed by the basic concepts and fundamental understanding of the reaction mechanisms, we present efficient strategies for the enhancement of the electrocatalytic performance of the catalysts to meet the rigorous requirement under industrial conditions and the in-depth understanding behind the reinforcement will be briefly discussed next. Then the recent advances regarding the rational design of electrocatalysts operating at an industrial scale will be summarized. Finally, the challenges and perspectives in this thriving field will be proposed from our point of view.展开更多
The development of efficient nonprecious bifunctional electrocatalysts for water electrolysis is crucial to enhance the sluggish kinetics of the oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).A sel...The development of efficient nonprecious bifunctional electrocatalysts for water electrolysis is crucial to enhance the sluggish kinetics of the oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).A self-supporting,multiscale porous NiFeZn/NiZn-Ni catalyst with a triple interface heterojunction on nickel foam(NF)(NiFeZn/NiZn-Ni/NF)was in-situ fabricated using an electroplating-annealing-etching strategy.The unique multiinterface engineering and three-dimensional porous scaffold significantly modify the mass transport and electron interaction,resulting in superior bifunctional electrocatalytic performance for water splitting.The NiFeZn/NiZn-Ni/NF catalyst demonstrates low overpotentials of 187 m V for HER and 320 mV for OER at a current density of 600 mA/cm^(2),along with high durability over 150 h in alkaline solution.Furthermore,an electrolytic cell assembled with NiFeZn/NiZn-Ni/NF as both the cathode and anode achieves the current densities of 600 and 1000 m A/cm^(2) at cell voltages of 1.796 and 1.901 V,respectively,maintaining the high stability at 50 mA/cm^(2) for over 100 h.These findings highlight the potential of NiFeZn/NiZn-Ni/NF as a cost-effective and highly efficient bifunctional electrocatalyst for overall water splitting.展开更多
Developing bifunctional electrocatalysts with both high catalytic activity and high stability is crucial for efficient water splitting in alkaline media.Herein,a Fe-incorporated dual-metal selenide on nickel foam(Co_(...Developing bifunctional electrocatalysts with both high catalytic activity and high stability is crucial for efficient water splitting in alkaline media.Herein,a Fe-incorporated dual-metal selenide on nickel foam(Co_(0.9)Fe_(0.1)-Se/NF) is synthesized via a facile one-step electrodeposition method.As-synthesized materials could serve as self-supported bifunctional electrocatalysts with excellent catalytic activity towards oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) in alkaline media.Experimental results show that delivering a 10 mA cm^(-2) water splitting current density only requires a cell voltage of 1.55 V.In addition,a very stable performance could be kept for about 36 hours,indicating their excellent working stability.Moreover,by means of phase analysis,we have identified that the evolution of the synthesized Co_(0.9)Fe_(0.1)-Se/NF experiences two entirely different processes in HER and OER,which hydroxide and oxyhydroxide are regarded as the real active sites,respectively.This work may pave the way to further understanding the relationships between the reactivity and stability of chalcogenide-based electrocatalysts and facilitating the rational design of efficient electrocatalysts for future renewable energy system applications.展开更多
The lamellar hydrates of CAC were designed with the introduction of nano CaCO_(3)or Mg-Al hydrotalcite(M-A-H),and the effects on the green strength,pore structures,and high-temperature fracture behavior of alumina-spi...The lamellar hydrates of CAC were designed with the introduction of nano CaCO_(3)or Mg-Al hydrotalcite(M-A-H),and the effects on the green strength,pore structures,and high-temperature fracture behavior of alumina-spinel castables were investigated.The results show that nano CaCO_(3)or M-A-H stimulates rapidly the hydration of CAC and the formation of lamellar C_(4)AcH_(11)or coexistence of C_(2)AH_(8)and C_(4)AcH_(11)at 25℃.The formation of lamellar hydrates can contribute to a more complicated pore structure,especially in the range of 400-2000 nm.Meanwhile,the incorporation of well-distributed CaO or MgO sources from nano CaCO_(3)or M-A-H also regulates the distribution of CA_(6)and spinel(pre-formed and in-situ).Consequently,the optimized microstructure and complicated pore structure can induce the deflection and bridging of cracks,thus facilitating the consumption of fracture energy and enhancing the resistance to thermal stress damage.展开更多
基金sponsored by the National Natural Science Foundation of China(Nos.5210125 and 52375422)the Science Research Project of Hebei Education Department(No.BJK2023058)the Natural Science Foundation of Hebei Province(Nos.E2020208069,B2020208083 and E202320801).
文摘The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.
基金financially supported by the National Natural Science Foundation of China(Nos.62001189 and 51802177)the Joint Funds of the National Natural Science Foundation of China(No.U22A20140)+2 种基金the Youth Innovation Group Plan of Shandong Province(No.2022KJ095)the Plan for the Introduction and Cultivation of Young Innovative Talent in the Colleges and Universities of Shandong ProvinceSupported by Guiding Fund of Zaozhuang Industrial Technology Research Institute of University of Jinan。
文摘To effectively address energy challenges,it is crucial to explore efficient and stable bifunctional nonprecious metal catalysts.In this study,a Mo-doped nickeliron layered double hydroxide with flower-cluster architecture was successfully prepared by a one-step hydrothermal method,which demonstrated a good water splitting performance.After an appropriate amount of Mo doping,some lattice distortions in the material provided reactive sites for the adsorption and conversion of intermediates,thus optimising the charge distribution of the material.Moreover,the multidimensional void structures formed after doping had a larger specific surface area and accelerated the penetration of the electrolyte,which significantly improved the activity of the catalyst in alkaline media.At 10 mA·cm^(-2),the hydrogen and oxygen evolution overpotentials of Mo-doped nickel-iron double hydroxides(Mo-NiFe LDH/NF-0.2)were 167 and 220 mV,respectively,with an excellent durability up to 24 h.When the Mo-NiFe LDH/NF-0,2 catalyst was used as the cathode and anode of an electrolytic cell,the catalyst achieved a current density of 10 mA·cm^(-2)at an applied voltage of 1.643 V.This study provides a novel approach for designing excellent bifunctional electrocatalysts containing nonprecious metals.
文摘Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic chlorine.Especially,it is full of challenges to unveil the key factors influencing the selectivity of such complex PEC processes.Herein,by regulating the energy band and surface structure of the anatase TiO_(2) nanotube array photoanode via nitrogen-doping,the seawater PEC oxidation shifts from Cl^(-)oxidation reaction(ClOR)dominant on the TiO_(2) photoanode(61.6%)to oxygen evolution reaction(OER)dominant on the N-TiO_(2) photoanode(62.9%).Comprehensive investigations including operando photoelectrochemical FTIR and DFT calculations unveil that the asymmetric hydrogen-bonding water at the N-TiO_(2) electrode/electrolyte interface enriches under illumination,facilitating proton transfer and moderate adsorption strength of oxygen-intermediates,which lowers the energy barrier for the OER yet elevates the energy barrier for the ClOR,resulting to a promoted selectivity towards the OER.The work sheds light on the underlying mechanism of the PEC water oxidation processes,and highlights the crucial role of interfacial water on the PEC selectivity,which could be regulated by controlling the energy band and the surface structure of semiconductors.
基金supported by the National Key R&D Program of China[Grant No.2023YFA1406304(J J)]the National Natural Science Foundation of China[Grant No.12174362(J J)]+2 种基金the Innovation Program for Quantum Science and Technology[Grant No.2021ZD0302803(D L F)]the New Cornerstone Science Foundation(D L F)Beamline 03U of the Shanghai Synchrotron Radiation Facility,which is supported by ME2 project under contract No.11227902 from the National Natural Science Foundation of China。
文摘Altermagnets represent a newly discovered class of magnetically ordered materials.Among all the candidates,CrSb stands out due to its largest spin splitting energy and highest Néel temperature exceeding 700 K,making it promising for room-temperature spintronic applications.Here we have successfully grown high quality CrSb(100)thin film on GaAs(110)substrate by molecular beam epitaxy.Using angle-resolved photoemission spectroscopy,we successfully obtained the three-dimensional electronic structure of the thin film.Moreover,we observed the emergence of the altermagnetic splitting bands corresponding to the calculated results along the low symmetry pathsT-QandP-D.The bands near the Fermi level are only spin splitting bands along theP-Ddirection,with splitting energy reaching as high as 910 meV.This finding provides insights into the magnetic properties of CrSb thin films and paves the way for further studies on their electronic structure and potential applications in spintronics.
基金supported by the National Natural Science Foundations of China(No.11972267 and 11802214)the Fundamental Research Funds for the Central Universities(No.104972024JYS0022)the Open Fund of the Hubei Longzhong Laboratory(No.2024KF-30).
文摘This study investigates the dynamic compressive behavior of three periodic lattice structures fabricated from Ti-6Al-4V titanium alloy,each with distinct topologies:simple cubic(SC),body-centered cubic(BCC),and face-centered cubic(FCC).Dynamic compression experiments were conducted using a Split Hopkinson Pressure Bar(SHPB)system,complemented by high-speed imaging to capture real-time deformation and failure mechanisms under impact loading.The influence of cell topology,relative density,and strain rate on dynamic mechanical properties,failure behavior,and stress wave propagation was systematically examined.Finite element modeling was performed,and the simulated results showed good agreement with experimental data.The findings reveal that the dynamic mechanical properties of the lattice structures are generally insensitive to strain rate variations,while failure behavior is predominantly governed by structural configuration.The SC structure exhibited strut buckling and instability-induced fracture,whereas the BCC and FCC structures displayed layer-by-layer crushing with lower strain rate sensitivity.Regarding stress wave propagation,all structures demonstrated significant attenuation capabilities,with the BCC structure achieving the greatest reduction in transmitted wave amplitude and energy.Across all configurations,wave reflection was identified as the primary energy dissipation mechanism.These results provide critical insights into the design of lattice structures for impact mitigation and energy absorption applications.
基金financially supported by the Natural Science Foundation of National(No.NSFC22208179)the Key Laboratory of Laser Technology and Optoelectronic Functional Materials of Hainan Province(No.2024LTOM05)
文摘This study,a core-shell CoPt@C assembled hierarchical catalyst(named CoPt@C)was prepared using a unique CH_(4)deposition strategy for highly efficient overall water splitting.CoPt@C is composed of dense CoPt@C core-shell nanoparticles(NPs)and a minor proportion of curled CoPt@nanotubes(CoPt@CNTs).Moreover,by adjusting the CH_(4)deposition time,the carbon shell thickness can be effectively regulated.Benefiting from the synergistic interaction between CoPt alloy and carbon shell,coupled with the high conductivity of the carbon shell,the overpotential of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)for CoPt@C is 15 and 120 mV at 10 mA cm^(-2).In addition,CoPt@C requires only 1.58 V to achieve 10 mA cm^(-2)for overall water splitting and maintains excellent stability over 80 h of continuous electrolysis.Density functional theory(DFT)calculations suggest that electrons transfer from the CoPt alloy NPs to the carbon shell,rendering the carbon shell electron-rich.Additionally,the hydrogen adsorption energy(ΔG*H)and the rate-determining step(ΔG*OOH)on CoPt@C are only-0.22 and 1.9 eV,respectively.
基金financially supported by the National Natural Science Foundation of China(No.51804216)。
文摘Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this work,we synthesized a self-supporting heterogeneous NiSe@Co_(0.85)Se/NF electrocatalyst using a facile in situ selenization of transition metal precursors that coated on the nickel foam(NF)in polyol solution.The NF was used as both conductive substrate and nickel source,ensuring superior electronic conductivity for catalyzing.The NiSe@-Co_(0.85)Se/NF exhibited remarkable bifunctional electrocatalytic activities with HER overpotential of 168 mV and OER overpotential of 258 mV to achieve 10 mA·cm-2.The water splitting system using NiSe@Co_(0.85)Se/NF as both anode and cathode electrodes achieved a current density of 10 mA·cm^(-2) at 1.61 V with nearly 100% faradaic efficiency and impressively long-term stability.The efficient bifunctional catalytic performance of NiSe@-Co_(0.85)Se/NF should be attributed to the electronic modulation and synergistic effect between NiSe and Co_(0.85)Se,the intrinsic metallic conductivity and the enlarged active sites exposure.This work provides a facile method for developing heterogeneous bifunctional catalysts for advanced electrochemical energy conversion technologies.
基金financially supported by the National Natural Science Foundation of China (Nos. 51874020 and 52004022)
文摘Stable non-noble metal bifunctional electrocatalysts are one of the challenges to the fluctuating overall water splitting driven by re-newable energy.Herein,a novel self-supporting hierarchically porous Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure as bifunctional electrocatalyst was constructed based on porous Ni-Fe electrodeposition on three-dimensional(3D)carbon fiber cloth,in situ oxidation,and chemical sulfuration.Results showed that the Ni_(x)Fe-S/NiFe_(2)O_(4) heterostructure with a large specific surface area exhibits good bifunctional activity and stability for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)because of the abundance of active sites,synergistic effect of the heterostructure,superhydrophilic surface,and stable,self-supporting structure.The results further confirmed that the Ni_(x)Fe-S phase in the heterostructure is transformed into metal oxides/hydroxides and Ni_(3)S_(2) during OER.Compared with the commercial 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer,the self-supporting Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) electrolyzer exhibits better stability and lower cell voltage in the fluctu-ating current density range of 10-500 mA/cm^(2).Particularly,the cell voltage of Ni1/5Fe-S/NiFe_(2)O_(4)||Ni1/2Fe-S/NiFe_(2)O_(4) is only approximately 3.91 V at an industrial current density of 500 mA/cm^(2),which is lower than that of the 20wt%Pt/C||IrO_(2)-Ta_(2)O_(5) electrolyzer(i.e.,approximately 4.79 V).This work provides a promising strategy to develop excellent bifunctional electrocatalysts for fluctuating overall water splitting.
基金Youth Innovation Promotion Association of the Chinese Academy of Sciences,Grant/Award Number:2021174National Natural Science Foundation of China,Grant/Award Number:51902326Natural Science Foundation of Shanxi Province,Grant/Award Numbers:201901D211588,20210302124421。
文摘Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of TMPs.Herein,a novel method for synthesizing CoP nanoparticles encapsu-lated in a rich-defect carbon shell(CoP/DCS)is developed through the self-assembly of modified polycyclic aromatic molecules.The graft and removal of high-activity C-N bonds of aromatic molecules render the controllable design of crystallite defects of carbon shell.The density functional theory calculation indicates that the carbon defects with unpaired electrons could effectively tailor the band structure of CoP.Benefiting from the improved activity and corrosion resistance,the CoP/DCS delivers outstanding difunctional hydrogen evolution reaction(88 mV)and oxygen evolution reaction(251 mV)performances at 10 mA cm^(−2)current density.Furthermore,the coupled water electrolyzer with CoP/DCS as both the cathode and anode presents ultralow cell voltages of 1.49 V to achieve 10 mA cm^(−2)with long-time stability.This strategy to improve TMPs electrocatalyst with rich-DCS and heterogeneous structure will inspire the design of other transition metal compound electrocatalysts for water splitting.
基金This work was financially supported by the National Key Research and Development Program of China(No.2016YFB0700300)the National Natural Science Foundation of China(Nos.51503014 and 51501008)the Fundamental Research Funds for the Central Universities of China(No.230201818-002A3).
文摘Photoelectrochemical(PEC) water splitting offers the capability of harvesting, storing, and converting solar energy into clean and sustainable hydrogen energy. Metal oxides are appealing photoelectrode materials because of their easy manufacturing and relatively high stability. In particular, metal oxides prepared by electrochemical anodization are typical of ordered nanostructures, which are beneficial for light harvesting, charge transfer and transport, and the adsorption and desorption of reactive species due to their high specific surface area and rich channels. However, bare anodic oxides still suffer from low charge separation and sunlight absorption efficiencies. Accordingly, many strategies of modifying anodic oxides have been explored and investigated. In this review, we attempt to summarize the recent advances in the rational design and modifications of these oxides from processes before, during, and after anodization. Rational design strategies are thoroughly addressed for each part with an aim to boost overall PEC performance. The ongoing efforts and challenges for future development of practical PEC electrodes are also presented.
基金supported by the National Natural Science Foundation of China(Grant Nos.11076009 and 11374062)the Chinese Association of Atomic and Molecular Data+1 种基金the Chinese National Fusion Project for ITER(Grant No.2015GB117000)the Leading Academic Discipline Project of Shanghai City,China(Grant No.B107)
文摘A comprehensive theoretical study of correlation effects on the fine-structure splitting within the ground configuration 3d9 of the Co-like HI45＋, Ta46＋, W47＋, and Au52＋ ions is performed by employing the multi-configuration Dirac-Hartree- Fock method in the active space approximation. It shows that the core-valence correlation with the inner-core 2p electron is more significant than with the outer 3p and 3s electrons, and the correlation with the 2s electron is also noticeable. The core-core correlation seems to be small and can be ignored. The calculated 2D3/2,5/2 splitting energies agree with the recent electron-beam ion-trap measurements [Phys. Rev. A 83 032517 （2011）, Eur. Phys. J. D 66 286 （2012）] to within the experimental uncertainties.
基金supported by the National Natural Science Foundation of China(Grant Nos.11274235 and 11104190)the Doctoral Education Fund of Education Ministry of China(Grant No.20110181120112)
文摘The inter-relation between zero-field splitting （ZFS） parameters and local lattice structures of the （CrSe4）6 clusters in ZnSe semiconductors has been established by using the complete diagonalization （of the energy matrix） method. On the basis of this, the local lattice distortions, the ZFS parameters D, a, F and the optical spectrum for Cr2＋ ions doped into ZnSe are theoretically investigated, and the contributions of the spin singlets have been taken into account. The calculated ZFS parameters are in good agreement with the experimental values. From our calculations, the tetragonal distortion parameters AR = 0.091A and Aθ = 4.28° of Cr2＋ in ZnSe are acquired, and the results suggest that there exists a tetragonal expansion distortion for the local lattice structure of （CrSe4）6- clusters in ZnSe crystals. The influence of the spin singlets on ZFS parameters is also discussed, indicating that the contributions to ZFS parameters a and F cannot be ignored.
基金supported by the Natural Science Foundation of Hebei Province(No.B2021208030)the College Students Innovation Training Program(Nos.202206224 and S2021113409001).
文摘Designing and synthesizing cost-effective bifunctional catalysts for overall alkaline water/seawater splitting is still a huge challenge for hydrogen production.Herein,Co/Ni/Fe/Mn based-amorphous high-entropy phosphoxide self-standing electrode(CNFMPO)is synthesized by the facile and fast electrodeposition method.CNFMPO exhibits excellent bifunctional electrocatalytic performances on alkaline water/seawater electrolysis.The hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)overpotentials of CNFMPO in alkaline water/seawater are as low as 43/73 and 252/282 mV to reach a current density of 10 mA cm^(-2),respectively.Additionally,two-electrode electrolyzers with CNFMPO||CNFMPO successfully achieve the current density of 10 mA cm^(-2) at low voltages of 1.54 and 1.56 V for overall alkaline water/seawater splitting,respectively.CNFMPO exhibits satisfactory long-term stability on overall alkaline water/seawater splitting for the surface reconstruction into active metal hydroxide/(oxy)hydroxide,phosphite,and phosphate.Moreover,no hypochlorite is detected during seawater electrolysis for the beneficial chlorite oxidation inhibition of the reconstructed phosphite and phosphate.The excellent catalytic performances of CNFMPO are due to the unique amorphous structure,multi-component synergistic effect,beneficial electronic structure modulation,and surface reconstruction during the catalytic reaction process.Therefore,CNFMPO has shown potential promotion to the development of the water/seawater splitting industry as a promising substituent for noble-metal electrocatalysts.This work provides new insights into the design of efficient bifunctional catalysts for overall water/seawater splitting.
基金supported by the Key projects of intergovernmental international cooperation in the Key R&D programs of the Ministry of Science and Technology of China(No.2021YFE0115800)the National Science Funding Committee of China(No.U20A20250)。
文摘Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and Au.The electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and HER.Impressively,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 V.Moreover,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was assembled.Accordingly,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS equipment.The interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.
基金the China Scholarship Council(CSC)for the financial support(202206230096)D.Yu would like to thank the CSC for the Doctor scholarship(202006360037)+1 种基金J.Dutta would like to acknowledge the partial financial support of VINNOVA project no.2021-02313.PZhang would like to acknowledge partial financial support from the National Natural Science Foundation of China(Nos 52111530187,51972210).
文摘Transition metal phosphides(TMPs)have emerged as an alternative to precious metals as efficient and low-cost catalysts for water electrolysis.Elemental doping and morphology control are effective approaches to further improve the performance of TMPs.Herein,Fe-doped CoP nanoframes(Fe-CoP NFs)with specific open cage configuration were designed and synthesized.The unique nano-framework structured Fe-CoP material shows overpotentials of only 255 and 122 mV at 10 mA cm^(−2)for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER),respectively,overwhelming most transition metal phosphides.For overall water splitting,the cell voltage is 1.65 V for Fe-CoP NFs at a current density of 10 mA cm^(−2),much superior to what is observed for the classical nanocubic structures.Fe-CoP NFs show no activity degradation up to 100 h which contrasts sharply with the rapidly decaying performance of noble metal catalyst reference.The superior electrocatalytic performance of Fe-CoP NFs due to abundant accessible active sites,reduced kinetic energy barrier,and preferable*O-containing intermediate adsorption is demonstrated through experimental observations and theoretical calculations.Our findings could provide a potential method for the preparation of multifunctional material with hollow structures and offer more hopeful prospects for obtaining efficient earth-abundant catalysts for water splitting.
基金Supported by Program for Changjiang Scholars and Innovative Research Team in University,Ministry of Education of China(PCSIRT)
文摘DC-inverter split air-conditioner is widely used in Chinese homes as a result of its high-efficiency and energy-saving. Recently, the researches on its outdoor unit have focused on the influence of surrounding structures upon the aerodynamic and acoustic performance, however they are only limited to the influence of a few parameters on the performance, and practical design of the unit requires more detailed parametric analysis. Three-dimensional computational fluid dynamics（CFD） and computational aerodynamic acoustics（CAA） simulation based on FLUENT solver is used to study the influence of surrounding structures upon the aforementioned properties of the unit. The flow rate and sound pressure level are predicted for different rotating speed, and agree well with the experimental results. The parametric influence of three main surrounding structures（i.e. the heat sink, the bell-mouth type shroud and the outlet grille） upon the aerodynamic performance of the unit is analyzed thoroughly. The results demonstrate that the tip vortex plays a major role in the flow fields near the blade tip and has a great effect on the flow field of the unit. The inlet ring＇s size and throat＇s depth of the bell-mouth type shroud, and the through-flow area and configuration of upwind and downwind sections of the outlet grille are the most important factors that affect the aerodynamic performance of the unit. Furthermore, two improved schemes against the existing prototype of the unit are developed, which both can significantly increase the flow rate more than 6 %（i.e. 100 m3·h～（-1）） at given rotating speeds. The inevitable increase of flow noise level when flow rate is increased and the advantage of keeping a lower rotating speed are also discussed. The presented work could be a useful guideline in designing the aerodynamic and acoustic performance of the split air-conditioner in engineering practice.
基金supported by the Program for Innovative Research Team in University of Henan Province(21IRTSTHN009)the Science and Technology Development Plan of Henan Province(212300410029,202300410087,202102210251)+2 种基金the Central Government of Shenzhen Guided the Local Science and Technology Exhibition Special Funds(2021Szvup031)the National Natural Science Foundation of China(52102166)the China Postdoctoral Science Foundation(2019M663058,2021M701065,2019M652749,2021M701071)。
文摘The green hydrogen generation powered by renewable electricity promises the potential decarbonization of the hard-to-abate sector and is essential for the fulfillment of the Paris Agreement that attempts to limit the global average temperature rise in the range of 1.5–2.0 ℃ above the pre-industrial level by the end of this century. Tremendous efforts have been devoted to the optimization of the electrocatalytic performance of the catalysts under industrial-relevant current densities via rational structure design,which induces a preferential electron distribution that favors the adsorption/desorption behavior of the key intermediates, thus accelerating the reaction kinetics. In this review, a brief introduction of the current energy status will be first presented to necessitate the importance of green hydrogen.Followed by the basic concepts and fundamental understanding of the reaction mechanisms, we present efficient strategies for the enhancement of the electrocatalytic performance of the catalysts to meet the rigorous requirement under industrial conditions and the in-depth understanding behind the reinforcement will be briefly discussed next. Then the recent advances regarding the rational design of electrocatalysts operating at an industrial scale will be summarized. Finally, the challenges and perspectives in this thriving field will be proposed from our point of view.
基金financially supported from the National Natural Science Foundation of China(No.52201254)the Natural Science Foundation of Shandong Province,China(Nos.ZR2023ME155,ZR2020MB090,ZR2020QE012,ZR2020MB027)+1 种基金the Project of“20 Items of University”of Jinan,China(No.202228046)the Taishan Scholar Project of Shandong Province,China(No.tsqn202306226)。
文摘The development of efficient nonprecious bifunctional electrocatalysts for water electrolysis is crucial to enhance the sluggish kinetics of the oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).A self-supporting,multiscale porous NiFeZn/NiZn-Ni catalyst with a triple interface heterojunction on nickel foam(NF)(NiFeZn/NiZn-Ni/NF)was in-situ fabricated using an electroplating-annealing-etching strategy.The unique multiinterface engineering and three-dimensional porous scaffold significantly modify the mass transport and electron interaction,resulting in superior bifunctional electrocatalytic performance for water splitting.The NiFeZn/NiZn-Ni/NF catalyst demonstrates low overpotentials of 187 m V for HER and 320 mV for OER at a current density of 600 mA/cm^(2),along with high durability over 150 h in alkaline solution.Furthermore,an electrolytic cell assembled with NiFeZn/NiZn-Ni/NF as both the cathode and anode achieves the current densities of 600 and 1000 m A/cm^(2) at cell voltages of 1.796 and 1.901 V,respectively,maintaining the high stability at 50 mA/cm^(2) for over 100 h.These findings highlight the potential of NiFeZn/NiZn-Ni/NF as a cost-effective and highly efficient bifunctional electrocatalyst for overall water splitting.
基金financial support from the National Natural Science Foundation of China (Grant Nos. 51972191, 51722207)。
文摘Developing bifunctional electrocatalysts with both high catalytic activity and high stability is crucial for efficient water splitting in alkaline media.Herein,a Fe-incorporated dual-metal selenide on nickel foam(Co_(0.9)Fe_(0.1)-Se/NF) is synthesized via a facile one-step electrodeposition method.As-synthesized materials could serve as self-supported bifunctional electrocatalysts with excellent catalytic activity towards oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) in alkaline media.Experimental results show that delivering a 10 mA cm^(-2) water splitting current density only requires a cell voltage of 1.55 V.In addition,a very stable performance could be kept for about 36 hours,indicating their excellent working stability.Moreover,by means of phase analysis,we have identified that the evolution of the synthesized Co_(0.9)Fe_(0.1)-Se/NF experiences two entirely different processes in HER and OER,which hydroxide and oxyhydroxide are regarded as the real active sites,respectively.This work may pave the way to further understanding the relationships between the reactivity and stability of chalcogenide-based electrocatalysts and facilitating the rational design of efficient electrocatalysts for future renewable energy system applications.
基金supported financially by the Natural Science Foundation of Qinghai(2022-ZJ-928)the Special Project for Transformation of Scientific and Technological Achievements of Qinghai Province(2023-GX-102).
文摘The lamellar hydrates of CAC were designed with the introduction of nano CaCO_(3)or Mg-Al hydrotalcite(M-A-H),and the effects on the green strength,pore structures,and high-temperature fracture behavior of alumina-spinel castables were investigated.The results show that nano CaCO_(3)or M-A-H stimulates rapidly the hydration of CAC and the formation of lamellar C_(4)AcH_(11)or coexistence of C_(2)AH_(8)and C_(4)AcH_(11)at 25℃.The formation of lamellar hydrates can contribute to a more complicated pore structure,especially in the range of 400-2000 nm.Meanwhile,the incorporation of well-distributed CaO or MgO sources from nano CaCO_(3)or M-A-H also regulates the distribution of CA_(6)and spinel(pre-formed and in-situ).Consequently,the optimized microstructure and complicated pore structure can induce the deflection and bridging of cracks,thus facilitating the consumption of fracture energy and enhancing the resistance to thermal stress damage.
