Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR cataly...Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations,ranging from single-atom,nanocluster to bulk Pt catalysts.The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale,and the Pt_(38)cluster had the lowest ORR overpotential(0.46 V)compared with that of Pt_(111)(0.57 V)and single atom Pt(0.7 V).Moreover,we established a volcano curve relationship between the ORR overpotential and binding energy of O*(ΔE_(O*),confirming the intermediate species anchored on Pt38cluster with suitable binding energy located at top of volcano curve.The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.展开更多
Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air cathode.Herein,a novel bimetallic Co/CoFe na...Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air cathode.Herein,a novel bimetallic Co/CoFe nanomaterial supported on nanoflower-like N-doped graphitic carbon(NC)was prepared through a strategy of coordination construction-cation exchange-pyrolysis and used as a highly efficient bifunctional oxygen electrocatalyst.Experimental characterizations and density functional theory calculations reveal the formation of Co/CoFe heterostructure and synergistic effect between metal layer and NC support,leading to improved electric conductivity,accelerated reaction kinetics,and optimized adsorption energy for intermediates of ORR and OER.The Co/CoFe@NC exhibits high bifunctional activities with a remarkably small potential gap of 0.70 V between the half-wave potential(E_(1/2))of ORR and the potential at 10 mA cm^(-2)(E_(j=10))of OER.The aqueous ZAB constructed using this air electrode exhibits a slight voltage loss of only 60 mV after 550-cycle test(360 h,15 days).A sodium polyacrylate(PANa)-based hydrogel electrolyte was synthesized with strong water-retention capability and high ionic conductivity.The quasi-solid-state ZAB by integrating the Co/CoFe@NC air electrode and PANa hydrogel electrolyte demonstrates excellent mechanical stability and cyclability under different bending states.展开更多
Rational design of highly efficient,robust and nonprecious electrocatalysts for the oxygen reduction reaction(ORR),oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is highly demanded and challenging.H...Rational design of highly efficient,robust and nonprecious electrocatalysts for the oxygen reduction reaction(ORR),oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is highly demanded and challenging.Here,heterostructural Co_(3O)_(4)@Ni_(2)P arrays with numerous reaction sites,unique interfacial electronic structure and fast charge transfer kinetics are developed as electrocatalysts for rechargeable Zn-air batteries and overall water splitting.Both density functional theory calculation and X-ray absorption fine structure analysis manifest that the synergistic structural and abundant electronic modulations interfaces are formed,thus simultaneously promoting the electrocatalytic kinetics,activities and stabilities.Specifically,it can achieve an ultralow overpotential of 270 m V and 28 m V at 10 m A cm^(-2) for OER and HER,respectively.The water electrolyzer delivers a current density of 10 m A cm^(-2) at 1.563 V;furthermore,rechargeable Zn-air batteries triggered by this heterostructure can achieve excellent cyclic stability of 177 h(2 h per cycle)at 10 m A cm^(-2);both devices are superior to the Pt/C+Ir/C.This work not only designs an efficient trifunctional electrocatalyst but also paves an avenue to understand the heterostructure engineering for catalysts development and disclose the underlying relationship of interfacial electronic structures and catalytic properties.展开更多
Subnanometer metal clusters play an increasingly important role in heterogeneous catalysis due to their high catalytic activity and selectivity.In this work,by means of the density functional theory(DFT) calculations,...Subnanometer metal clusters play an increasingly important role in heterogeneous catalysis due to their high catalytic activity and selectivity.In this work,by means of the density functional theory(DFT) calculations,the catalytic activities of transition metal clusters with precise numbers of atoms supported on graphdiyne(TM_(1-4)@GDY,TM=V,Cr,Mn,Fe,Co,Ni,Cu,Ru,Rh,Pd,Ir,Pt) were investigated for oxygen evolution reactions(OER),oxygen reduction reactions(ORR) and hydrogen evolution reactions(HER).The computed results reveal that the Pd_(2),Pd_(4) and Pt_(1) anchored graphdiyne can serve as trifunctional catalysts for OER/ORR/HER with the overpotentials of 0.49/0.37/0.06,0.45/0.33/0.12 and 0.37/0.43/0.01 V,respectively,while Pd_(1) and Pt_(2)@graphdiyne can exhibit excellent catalytic performance for water splitting(OER/HER) with the overpotentials of 0.55/0.17 and 0.43/0.03 V.In addition,Ni_(1) and Pd_(3) anchored GDY can perform as bifunctional catalysts for metal-air cells(OER/ORR) and fuels cells(ORR/HER) with the overpotentials of 0.34/0.32 and 0.42/0.04 V,respectively.Thus,by precisely controlling the numbers of atoms in clusters,the TM_(1-4) anchored graphdiyne can serve as promising multifunctional electrocatalysts for OER/ORR/HER,which may provide an instructive strategy to design catalysts for the energy conversation and storage devices.展开更多
The electrochemical nitrogen reduction reaction(NRR)for the ammonia production under ambient conditions is regarded as a sustainable alternative to the industrial Haber-Bosch process.However,the electrocatalytic syste...The electrochemical nitrogen reduction reaction(NRR)for the ammonia production under ambient conditions is regarded as a sustainable alternative to the industrial Haber-Bosch process.However,the electrocatalytic systems that efficiently catalyze nitrogen reduction remain elusive.In the work,the nitrogen reduction activity of the transition metal decorated bismuthene TM@Bis is fully investigated by means of density functional theory calculations.Our results demonstrate that W@Bis delivers the best efficiency,wherein the potential-determining step is located at the last protonation step of^(*)NH_(2)+H^(+)+e^(-)→*NH_(3)via the distal mechanism with the limiting potential ULof 0.26 V.Furthermore,the dopants of Re and Os are also promising candidates for experimental synthesis due to its good selectivity,in despite of the slightly higher ULof NRR with the value of 0.55 V.However,the candidates of Ti,V,Nb and Mo delivered the relative lower ULof 0.35,0.37,0.41 and 0.43 V might be suffered from the side hydrogen evolution reaction.More interestingly,a volcano curve is established between ULand valence electrons of metal elements wherein W with 4 electrons in d band located at the summit.Such phenomenon originates from the underlying acceptance-back donation mechanism.Therefore,our work provides a fundament understanding for the material design for nitrogen reduction electrocatalysis.展开更多
Green hydrogen production and CO_(2) fixation have been identified as the fundamental techniques for sustainable economy.The open challenge is to develop high performance catalysts for hydrogen evolution reaction(HER)...Green hydrogen production and CO_(2) fixation have been identified as the fundamental techniques for sustainable economy.The open challenge is to develop high performance catalysts for hydrogen evolution reaction(HER)and CO_(2) electroreduction(CO_(2)ER)to valuable chemicals.Under such context,this work reported computational efforts to design promising electrocatalyst for HER and CO_(2)ER based on the swarm-intelligence algorithm.Among the family of transition-metal phosphides(TMPs),Pt_(2)P_(3) monolayer has been identified as excellent bifunctional catalysts due to high stability,excellent conductivity and superior catalytic performance.Different from typical d-block catalysts,p-band center presented by P atoms within Pt_(2)P_(3) monolayer plays the essential role for its reactivity towards HER and CO_(2)ER,underlining the key value of p-electrons in advanced catalyst design and thus providing a promising strategy to further develop novel catalysts made of p-block elements for various energy applications.展开更多
The exploitation of cost-efficient electrocatalysts is critical to develop the hydrogen evolution reaction(HER) for hydrogen production.Herein,Ni_(3)S_(2)/NF-x h(x=12,16 and 20,reaction time) nanocrystals in-situ grow...The exploitation of cost-efficient electrocatalysts is critical to develop the hydrogen evolution reaction(HER) for hydrogen production.Herein,Ni_(3)S_(2)/NF-x h(x=12,16 and 20,reaction time) nanocrystals in-situ grown on Ni foam(NF) were prepared via a facile hydrothermal method.The results demonstrate that the reaction time plays key roles in the morphology,the hydrogen evolution performance of the samples,and the hydrogen brittleness of NF substrate.Interestingly,the Ni_(3)S_(2)/NF-16 h displays outstanding catalytic activity for HER in alkaline solution and avoids the hydrogen brittleness of the NF skeletons simultaneously.To afford a catalytic current of20 mA·cm^(-2),Ni_(3)S_(2)/NF-16 h presents ultra-low overpotential of 48 mV for hydrogen evolution and sufficient stability for 40 h.Moreover,the density functional theory(DFT) calculations revealed that the excellent electrocatalytic HER activity of Ni_(3)S_(2) could be attributed to its exposed(015) plane,which exhibited good capability for water adsorption and dissociation in an alkaline electrolyte,leading to the optimal free energy for H^(*) adsorption.The present work offers a novel strategy to design,synthesize and develop highly efficient electrocatalysts for HER.展开更多
In this paper,we report,for the first time,on the electrochemical catalytic activity of 2D titanium carbonitride MXene for hydrogen evolution reaction(HER).According to our study,2D titanium carbonitride exhibited muc...In this paper,we report,for the first time,on the electrochemical catalytic activity of 2D titanium carbonitride MXene for hydrogen evolution reaction(HER).According to our study,2D titanium carbonitride exhibited much higher electrocatalytic activity than its carbide analogues,achieving an onset overpotential of 53 mV and Tafel slope of 86 mV dec^(-1),superior to the titanium carbide with onset overpotential of 649 mV and Tafel slope of 303 mV dec^(-1).The obtained onset overpotential for 2D titanium carbonitride is lower than those of all the reported transition metal carbides MXene catalysts without additives,so far.Density functional theory calculations were conducted to further understand the electrochemical performance.The calculation results show that a greater number of occupied states are active for Ti_(3)CNO_(2),revealing free energy for the adsorption of atomic hydrogen closer to 0 than that of Ti_(3)C_(2)O_(2).Both experimental and calculation studies demonstrate the excellent electrocatalytic behavior of titanium carbonitride.The investigation of 2D titanium carbonitride opens up a promising paradigm for the conscious design of high-performance non-precious metal catalyst for hydrogen generation.展开更多
The development of stable and highly efficien multifunctional electrocatalysts for the hydrogen evolution reaction(HER),oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are essential for the efficient c...The development of stable and highly efficien multifunctional electrocatalysts for the hydrogen evolution reaction(HER),oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are essential for the efficient conversion and storage of renewable energy.The significant advantages of single-atom catalysts,such as strong metal slab interactions,unsaturated coordination and efficient atomic utilization,have opened new avenues for designing multifunctional catalysts.Herein,based on density functional theory,a single atom doped PdPX system was designed as a multifunctional electrocatalyst,which demonstrated the synergistic effect between defects and transition metal atoms and led to enhanced catalytic performance.The results showed that PdPS/PdPSe with P/X vacancy,PdPTe with P/Pd vacancy and Co/Rh/Ir@PdPX exhibited promising HER activity.Co@PdPS(Se),with an overpotential of 0.56(0.44)V,was predicted to be a promising OER catalyst.Moreover,Rh(Ir)@PdPS(Se)catalysts exhibited efficient catalytic properties for ORR Besides,Co@PdPS(Se),Rh(Ir)@PdPS~(V(S)),Co@PdP-Se~(V(Se))and Ir@PdPS~(V(S)-1)exihibited multifunctional catalytic performance with moderate overpotential.Next,the origin of catalytic activity was revealed by using the crystal orbital Hamilton populations theory.For a strong adsorption system,proper filling of the anti-bonding state can increase the energy of the system,weaken the adsorption strength,and facilitate the desorption of intermediates Conversely,augmenting bonding states can enhance its adsorption capacity.These findings provide theoretica guidance for the design and fabrication of novel multifunctional electrocatalysts in terms of filling of bondingstate.展开更多
Phase engineering is an efficient strategy for enhancing the kinetics of electrocatalytic reactions.Herein,phase engineering was employed to prepare high‐performance phosphorous‐doped biphase(1T/2H)MoS_(2)(P‐BMS)na...Phase engineering is an efficient strategy for enhancing the kinetics of electrocatalytic reactions.Herein,phase engineering was employed to prepare high‐performance phosphorous‐doped biphase(1T/2H)MoS_(2)(P‐BMS)nanoflakes for hydrogen evolution reaction(HER).The doping of MoS_(2)with P atoms modifies its electronic structure and optimizes its electrocatalytic reaction kinetics,which significantly enhances its electrical conductivity and structural stability,which are verified by various characterization tools,including X‐ray photoelectron spectroscopy,high‐resolution transmission electron microscopy,X‐ray absorption near‐edge spectroscopy,and extended X‐ray absorption fine structure.Moreover,the hierarchically formed flakes of P‐BMS provide numerous catalytic surface‐active sites,which remarkably enhance its HER activity.The optimized P‐BMS electrocatalysts exhibit low overpotentials(60 and 72 mV at 10 mA cm^(−2))in H_(2)SO_(4)(0.5 M)and KOH(1.0 M),respectively.The mechanism of improving the HER activity of the material was systematically studied using density functional theory calculations and various electrochemical characterization techniques.This study has shown that phase engineering is a promising strategy for enhancing the H*adsorption of metal sulfides.展开更多
The strategic manipulation of the interaction between a central metal atom and its coordinating environment in single-atom catalysts(SACs)is crucial for catalyzing the CO_(2)reduction reaction(CO_(2)RR).However,it rem...The strategic manipulation of the interaction between a central metal atom and its coordinating environment in single-atom catalysts(SACs)is crucial for catalyzing the CO_(2)reduction reaction(CO_(2)RR).However,it remains a major challenge.While density-functional theory calculations serve as a powerful tool for catalyst screening,their time-consuming nature poses limitations.This paper presents a machine learning(ML)model based on easily accessible intrinsic descriptors to enable rapid,cost-effective,and high-throughput screening of efficient SACs in complex systems.Our ML model comprehensively captures the influences of interactions between 3 and 5d metal centers and 8 C,N-based coordination environments on CO_(2)RR activity and selectivity.We reveal the electronic origin of the different activity trends observed in early and late transition metals during coordination with N atoms.The extreme gradient boosting regression model shows optimal performance in predicting binding energy and limiting potential for both HCOOH and CO production.We confirm that the product of the electronegativity and the valence electron number of metals,the radius of metals,and the average electronegativity of neighboring coordination atoms are the critical intrinsic factors determining CO_(2)RR activity.Our developed ML models successfully predict several high-performance SACs beyond the existing database,demonstrating their potential applicability to other systems.This work provides insights into the low-cost and rational design of high-performance SACs.展开更多
The practical application of Lithium-Sulfur batteries largely depends on highly efficient utilization and conversion of sulfur under the realistic condition of high-sulfur content and low electrolyte/sulfur ratio.Rati...The practical application of Lithium-Sulfur batteries largely depends on highly efficient utilization and conversion of sulfur under the realistic condition of high-sulfur content and low electrolyte/sulfur ratio.Rational design of heterostructure electrocatalysts with abundant active sites and strong interfacial electronic interactions is a promising but still challenging strategy for preventing shuttling of polysulfides in lithium-sulfur batteries.Herein,ultrathin nonlayered NiO/Ni_(3)S_(2)heterostructure nanosheets are developed through topochemical transformation of layered Ni(OH)_(2)templates to improve the utilization of sulfur and facilitate stable cycling of batteries.As a multifunction catalyst,NiO/Ni_(3)S_(2)not only enhances the adsorption of polysulfides and shorten the transport path of Li ions and electrons but also promotes the Li_(2)S formation and transformation,which are verified by both in-situ Raman spectroscopy and electrochemical investigations.Thus,the cell with NiO/Ni_(3)S_(2)as electrocatalyst delivers an area capacity of 4.8 mAh cm^(-2)under the high sulfur loading(6 mg cm^(-2))and low electrolyte/sulfur ratio(4.3 pL mg^(-1)).The strategy can be extended to 2D Ni foil,demonstrating its prospects in the construction of electrodes with high gravimetric/volumetric energy densities.The designed electrocatalyst of ultrathin nonlayered heterostructure will shed light on achieving high energy density lithium-sulfur batteries.展开更多
Recently,metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications.The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic clus...Recently,metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications.The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory.Firstly,the catalytic activities of heterometallic clusters are investigated.Among all heterometallic clusters,Fe_(2)Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction,and Fe_(2)Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction,respectively 100 and 50 mV lower than those of Pt(111)and RuO_(2)(110)catalysts.The analysis of the potential gap of Fe_(2)M clusters indicates that Fe_(2)Mn,Fe_(2)Co,and Fe_(2)Ni clusters possess good bifunctional catalytic activity.Additionally,the catalytic activity of Fe_(2)Mn and Fe_(2)Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe_(2)M–PCN–Fe_(2)M is explored.Compared with Fe_(2)Mn–PCN–Fe_(2)Mn,Fe_(2)Co–PCN–Fe_(2)Co,and isolated Fe_(2)M clusters,the mixed-metal Fe_(2)Co–PCN–Fe_(2)Mn possesses excellent bifunctional catalytic activity,and the values of potential gap on the Mn and Co sites of Fe_(2)Co–PCN–Fe_(2)Mn are 0.69 and 0.70 V,respectively.Furthermore,the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst.In conclusion,the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.展开更多
Self-supporting electrocatalysts for the oxygen evolution reaction(OER)require a delicate balance of cost-effectiveness,high activity,substantial durability,and robust mechanical properties.Here,we leverage the chemic...Self-supporting electrocatalysts for the oxygen evolution reaction(OER)require a delicate balance of cost-effectiveness,high activity,substantial durability,and robust mechanical properties.Here,we leverage the chemical and structural complexity of Al_(16.7) Fe_(16.7) Co_(16.7) Ni_(16.7) Cr_(16.7) Mn_(16.7)(at.%)high-entropy alloy(HEA)to address these requirements.Utilizing spinodal decomposition,we achieve a nanoporous structure of Fe-Cr-rich phase(A2 phase),providing a large specific surface area and robust mechanical integrity for free-standing applications.During cyclic voltammetry(CV)activation,an amorphous Mn-Fe-based HEA oxide forms in-situ on the nanoporous A2 phase,serving as an efficient electrocatalyst for OER in alkaline conditions.This nanoporous HEA amorphous oxide catalyst exhibits a low overpotential of 238 mV at a current density of 10 mA cm^(-2) and a low Tafel slope of 46 mV dec^(-1),surpassing the state-of-the-art RuO_(2) catalyst.This study establishes a competitive,engineering-applicable OER electrocatalyst and underscores the high-entropy effect’s potential in tuning electronic structures for enhanced performance.展开更多
Developing NO_(2)−reduction reaction(NO_(2)−RR)and oxygen evolution reaction(OER)bifunctional electrocatalysts at large current densities is crucial for decreasing energy consumption of electrocatalytic NH3 production...Developing NO_(2)−reduction reaction(NO_(2)−RR)and oxygen evolution reaction(OER)bifunctional electrocatalysts at large current densities is crucial for decreasing energy consumption of electrocatalytic NH3 production and booming sustainable nitrogenbased economy.In addition to increasing active sites of catalysts,bubble adhesion deserves more attention during high-current electrolysis,which can deteriorate mass transfer and block active sites in gas-involving environments.Herein,super-hydrophilic/aerophobic cobalt-nickel-iron layered double hydroxide[Co(OH)_(2)/NiFe LDH]core-shell heterostructures were developed as efficient NO_(2)−RR and OER electrocatalysts to optimize surface tension due to self-pumping effect and modify active hydrogen adsorption behavior owing to moderate work function difference between Co(OH)_(2)and NiFe LDH.The fabricated Co(OH)_(2)/NiFe LDH exhibited excellent NO_(2)−RR activity(yield:50 mg h^(−1)cm^(−2);FE:91%at−500 mA cm^(−2))and impressive OER behavior(η1000:340 mV)accompanied by remarkable application potential for renewable energy-driven two-electrode system to produce NH3.This effort revealed important insights into the development of electrodes for reaching cost-effective electrocatalytic ammonia production at large current densities.展开更多
Hydrogen generation and related energy applications heavily rely on the hydrogen evolution reaction(HER),which faces challenges of slow kinetics and high overpotential.Efficient electrocatalysts,particularly single-at...Hydrogen generation and related energy applications heavily rely on the hydrogen evolution reaction(HER),which faces challenges of slow kinetics and high overpotential.Efficient electrocatalysts,particularly single-atom catalysts (SACs) on two-dimensional (2D) materials,are essential.This study presents a few-shot machine learning (ML) assisted high-throughput screening of 2D septuple-atomic-layer Ga_(2)CoS_(4-x)supported SACs to predict HER catalytic activity.Initially,density functional theory (DFT)calculations showed that 2D Ga_(2)CoS4is inactive for HER.However,defective Ga_(2)CoS_(4-x)(x=0–0.25)monolayers exhibit excellent HER activity due to surface sulfur vacancies (SVs),with predicted overpotentials (0–60 mV) comparable to or lower than commercial Pt/C,which typically exhibits an overpotential of around 50 m V in the acidic electrolyte,when the concentration of surface SV is lower than 8.3%.SVs generate spin-polarized states near the Fermi level,making them effective HER sites.We demonstrate ML-accelerated HER overpotential predictions for all transition metal SACs on 2D Ga_(2)CoS_(4-x).Using DFT data from 18 SACs,an ML model with high prediction accuracy and reduced computation time was developed.An intrinsic descriptor linking SAC atomic properties to HER overpotential was identified.This study thus provides a framework for screening SACs on 2D materials,enhancing catalyst design.展开更多
Defect engineering has been used to develop low-cost and effective catalysts to boost oxygen reduction reactions.However,the development of catalysts that use metal cation vacancies as the active sites for oxygen redu...Defect engineering has been used to develop low-cost and effective catalysts to boost oxygen reduction reactions.However,the development of catalysts that use metal cation vacancies as the active sites for oxygen reduction reaction is lacking.In this study,ZnS nanoparticles on N-doped carbon serve as an oxygen reduction reaction catalyst.These catalysts were prepared via a one-step method at 900℃.Amazingly,the high-resolution transmission electron microscope image revealed obvious defects in the ZnS nanoparticles.These facilitated the catalyst synthesis,and the product displayed good electrocatalytic performance for the oxygen reduction reaction in an alkaline medium,including a lower onset potential,lower mid-wave potential,four electron transfer process,and better durability compared with 20 wt%Pt/C.More importantly,the density functional theory results indicated that using the Zn vacancies in the prepared catalyst as active sites required a lower reaction energy to produce OOH*from*OO toward oxygen reduction reaction.Therefore,the proposed catalyst with Zn vacancies can be used as a potential electrocatalyst and may be substitutes for Pt-based catalysts in fuel cells,given the novel catalyst’s resulting performance.展开更多
基金supported by the National Natural Science Foundation of China(92061125,21978294)Beijing Natural Science Foundation(Z200012)+3 种基金Jiangxi Natural Science Foundation(20212ACB213009)DNL Cooperation Fund,CAS(DNL201921)Self-deployed Projects of Ganjiang Innovation Academy,Chinese Academy of Sciences(E055B003)Hebei Natural Science Foundation(B2020103043)。
文摘Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations,ranging from single-atom,nanocluster to bulk Pt catalysts.The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale,and the Pt_(38)cluster had the lowest ORR overpotential(0.46 V)compared with that of Pt_(111)(0.57 V)and single atom Pt(0.7 V).Moreover,we established a volcano curve relationship between the ORR overpotential and binding energy of O*(ΔE_(O*),confirming the intermediate species anchored on Pt38cluster with suitable binding energy located at top of volcano curve.The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.
基金This work was supported by the National Natural Science Foundation of China(21872105,22072107)the Science&Technology Commission of Shanghai Municipality(19DZ2271500).
文摘Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air cathode.Herein,a novel bimetallic Co/CoFe nanomaterial supported on nanoflower-like N-doped graphitic carbon(NC)was prepared through a strategy of coordination construction-cation exchange-pyrolysis and used as a highly efficient bifunctional oxygen electrocatalyst.Experimental characterizations and density functional theory calculations reveal the formation of Co/CoFe heterostructure and synergistic effect between metal layer and NC support,leading to improved electric conductivity,accelerated reaction kinetics,and optimized adsorption energy for intermediates of ORR and OER.The Co/CoFe@NC exhibits high bifunctional activities with a remarkably small potential gap of 0.70 V between the half-wave potential(E_(1/2))of ORR and the potential at 10 mA cm^(-2)(E_(j=10))of OER.The aqueous ZAB constructed using this air electrode exhibits a slight voltage loss of only 60 mV after 550-cycle test(360 h,15 days).A sodium polyacrylate(PANa)-based hydrogel electrolyte was synthesized with strong water-retention capability and high ionic conductivity.The quasi-solid-state ZAB by integrating the Co/CoFe@NC air electrode and PANa hydrogel electrolyte demonstrates excellent mechanical stability and cyclability under different bending states.
基金the National Natural Science Foundation of China(Nos.22179014 and 21603019)the Fundamental Research Funds for the Central Universities(No.2021CDJQY-051)+1 种基金the Key Program for International Science and Technology Cooperation Projects of Ministry of Science and Technology of China(No.2016YFE0125900)the Hundred Talents Program of Chongqing University。
文摘Rational design of highly efficient,robust and nonprecious electrocatalysts for the oxygen reduction reaction(ORR),oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is highly demanded and challenging.Here,heterostructural Co_(3O)_(4)@Ni_(2)P arrays with numerous reaction sites,unique interfacial electronic structure and fast charge transfer kinetics are developed as electrocatalysts for rechargeable Zn-air batteries and overall water splitting.Both density functional theory calculation and X-ray absorption fine structure analysis manifest that the synergistic structural and abundant electronic modulations interfaces are formed,thus simultaneously promoting the electrocatalytic kinetics,activities and stabilities.Specifically,it can achieve an ultralow overpotential of 270 m V and 28 m V at 10 m A cm^(-2) for OER and HER,respectively.The water electrolyzer delivers a current density of 10 m A cm^(-2) at 1.563 V;furthermore,rechargeable Zn-air batteries triggered by this heterostructure can achieve excellent cyclic stability of 177 h(2 h per cycle)at 10 m A cm^(-2);both devices are superior to the Pt/C+Ir/C.This work not only designs an efficient trifunctional electrocatalyst but also paves an avenue to understand the heterostructure engineering for catalysts development and disclose the underlying relationship of interfacial electronic structures and catalytic properties.
基金financially supported by Fundamental Research Funds for Heilongjiang Province universities (No.2021-KYYWF-0184)Harbin Normal University Graduate Student Innovation Project (No.HSDSSCX2023-30)。
文摘Subnanometer metal clusters play an increasingly important role in heterogeneous catalysis due to their high catalytic activity and selectivity.In this work,by means of the density functional theory(DFT) calculations,the catalytic activities of transition metal clusters with precise numbers of atoms supported on graphdiyne(TM_(1-4)@GDY,TM=V,Cr,Mn,Fe,Co,Ni,Cu,Ru,Rh,Pd,Ir,Pt) were investigated for oxygen evolution reactions(OER),oxygen reduction reactions(ORR) and hydrogen evolution reactions(HER).The computed results reveal that the Pd_(2),Pd_(4) and Pt_(1) anchored graphdiyne can serve as trifunctional catalysts for OER/ORR/HER with the overpotentials of 0.49/0.37/0.06,0.45/0.33/0.12 and 0.37/0.43/0.01 V,respectively,while Pd_(1) and Pt_(2)@graphdiyne can exhibit excellent catalytic performance for water splitting(OER/HER) with the overpotentials of 0.55/0.17 and 0.43/0.03 V.In addition,Ni_(1) and Pd_(3) anchored GDY can perform as bifunctional catalysts for metal-air cells(OER/ORR) and fuels cells(ORR/HER) with the overpotentials of 0.34/0.32 and 0.42/0.04 V,respectively.Thus,by precisely controlling the numbers of atoms in clusters,the TM_(1-4) anchored graphdiyne can serve as promising multifunctional electrocatalysts for OER/ORR/HER,which may provide an instructive strategy to design catalysts for the energy conversation and storage devices.
基金the financial support from the National Natural Science Foundation of China(Nos.21503097,52130101,51701152,21806023 and 51702345)China Scholarship Council(No.202008320215)。
文摘The electrochemical nitrogen reduction reaction(NRR)for the ammonia production under ambient conditions is regarded as a sustainable alternative to the industrial Haber-Bosch process.However,the electrocatalytic systems that efficiently catalyze nitrogen reduction remain elusive.In the work,the nitrogen reduction activity of the transition metal decorated bismuthene TM@Bis is fully investigated by means of density functional theory calculations.Our results demonstrate that W@Bis delivers the best efficiency,wherein the potential-determining step is located at the last protonation step of^(*)NH_(2)+H^(+)+e^(-)→*NH_(3)via the distal mechanism with the limiting potential ULof 0.26 V.Furthermore,the dopants of Re and Os are also promising candidates for experimental synthesis due to its good selectivity,in despite of the slightly higher ULof NRR with the value of 0.55 V.However,the candidates of Ti,V,Nb and Mo delivered the relative lower ULof 0.35,0.37,0.41 and 0.43 V might be suffered from the side hydrogen evolution reaction.More interestingly,a volcano curve is established between ULand valence electrons of metal elements wherein W with 4 electrons in d band located at the summit.Such phenomenon originates from the underlying acceptance-back donation mechanism.Therefore,our work provides a fundament understanding for the material design for nitrogen reduction electrocatalysis.
基金financially supported by the Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province(No.JC2018004)the National Natural Science Foundation of China(No.11964024)+2 种基金the“Grassland Talents”project of Inner Mongolia autonomous region(No.12000-12102613)the Young science and technology talents cultivation project of Inner Mongolia University(No.21221505)supported by Harbin Normal University and Beijing Paratera Technology Co.,Ltd。
文摘Green hydrogen production and CO_(2) fixation have been identified as the fundamental techniques for sustainable economy.The open challenge is to develop high performance catalysts for hydrogen evolution reaction(HER)and CO_(2) electroreduction(CO_(2)ER)to valuable chemicals.Under such context,this work reported computational efforts to design promising electrocatalyst for HER and CO_(2)ER based on the swarm-intelligence algorithm.Among the family of transition-metal phosphides(TMPs),Pt_(2)P_(3) monolayer has been identified as excellent bifunctional catalysts due to high stability,excellent conductivity and superior catalytic performance.Different from typical d-block catalysts,p-band center presented by P atoms within Pt_(2)P_(3) monolayer plays the essential role for its reactivity towards HER and CO_(2)ER,underlining the key value of p-electrons in advanced catalyst design and thus providing a promising strategy to further develop novel catalysts made of p-block elements for various energy applications.
基金financially supported by the Project of Talent Recruitment of Guangdong University of Petrochemical Technology (Nos. 2019rc052 and 2019rc054)。
文摘The exploitation of cost-efficient electrocatalysts is critical to develop the hydrogen evolution reaction(HER) for hydrogen production.Herein,Ni_(3)S_(2)/NF-x h(x=12,16 and 20,reaction time) nanocrystals in-situ grown on Ni foam(NF) were prepared via a facile hydrothermal method.The results demonstrate that the reaction time plays key roles in the morphology,the hydrogen evolution performance of the samples,and the hydrogen brittleness of NF substrate.Interestingly,the Ni_(3)S_(2)/NF-16 h displays outstanding catalytic activity for HER in alkaline solution and avoids the hydrogen brittleness of the NF skeletons simultaneously.To afford a catalytic current of20 mA·cm^(-2),Ni_(3)S_(2)/NF-16 h presents ultra-low overpotential of 48 mV for hydrogen evolution and sufficient stability for 40 h.Moreover,the density functional theory(DFT) calculations revealed that the excellent electrocatalytic HER activity of Ni_(3)S_(2) could be attributed to its exposed(015) plane,which exhibited good capability for water adsorption and dissociation in an alkaline electrolyte,leading to the optimal free energy for H^(*) adsorption.The present work offers a novel strategy to design,synthesize and develop highly efficient electrocatalysts for HER.
基金supported by Tulane University.M.K.acknowledges the support by the US Department of Energy under EPSCoR Grant No.DE-SC0012432 with additional support from the Louisiana Board of Regents.
文摘In this paper,we report,for the first time,on the electrochemical catalytic activity of 2D titanium carbonitride MXene for hydrogen evolution reaction(HER).According to our study,2D titanium carbonitride exhibited much higher electrocatalytic activity than its carbide analogues,achieving an onset overpotential of 53 mV and Tafel slope of 86 mV dec^(-1),superior to the titanium carbide with onset overpotential of 649 mV and Tafel slope of 303 mV dec^(-1).The obtained onset overpotential for 2D titanium carbonitride is lower than those of all the reported transition metal carbides MXene catalysts without additives,so far.Density functional theory calculations were conducted to further understand the electrochemical performance.The calculation results show that a greater number of occupied states are active for Ti_(3)CNO_(2),revealing free energy for the adsorption of atomic hydrogen closer to 0 than that of Ti_(3)C_(2)O_(2).Both experimental and calculation studies demonstrate the excellent electrocatalytic behavior of titanium carbonitride.The investigation of 2D titanium carbonitride opens up a promising paradigm for the conscious design of high-performance non-precious metal catalyst for hydrogen generation.
基金financially supported by the National Natural Science Foundation of China(No.12204215)Shandong Provincial Natural Science Foundation,China(Nos.ZR2022ME030 and ZR2021QA026)。
文摘The development of stable and highly efficien multifunctional electrocatalysts for the hydrogen evolution reaction(HER),oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are essential for the efficient conversion and storage of renewable energy.The significant advantages of single-atom catalysts,such as strong metal slab interactions,unsaturated coordination and efficient atomic utilization,have opened new avenues for designing multifunctional catalysts.Herein,based on density functional theory,a single atom doped PdPX system was designed as a multifunctional electrocatalyst,which demonstrated the synergistic effect between defects and transition metal atoms and led to enhanced catalytic performance.The results showed that PdPS/PdPSe with P/X vacancy,PdPTe with P/Pd vacancy and Co/Rh/Ir@PdPX exhibited promising HER activity.Co@PdPS(Se),with an overpotential of 0.56(0.44)V,was predicted to be a promising OER catalyst.Moreover,Rh(Ir)@PdPS(Se)catalysts exhibited efficient catalytic properties for ORR Besides,Co@PdPS(Se),Rh(Ir)@PdPS~(V(S)),Co@PdP-Se~(V(Se))and Ir@PdPS~(V(S)-1)exihibited multifunctional catalytic performance with moderate overpotential.Next,the origin of catalytic activity was revealed by using the crystal orbital Hamilton populations theory.For a strong adsorption system,proper filling of the anti-bonding state can increase the energy of the system,weaken the adsorption strength,and facilitate the desorption of intermediates Conversely,augmenting bonding states can enhance its adsorption capacity.These findings provide theoretica guidance for the design and fabrication of novel multifunctional electrocatalysts in terms of filling of bondingstate.
基金National Natural Science Foundation of China,Grant/Award Number:NSFC‐U1904215National Research Foundation of Korea,Grant/Award Number:2021R1A2C2012127。
文摘Phase engineering is an efficient strategy for enhancing the kinetics of electrocatalytic reactions.Herein,phase engineering was employed to prepare high‐performance phosphorous‐doped biphase(1T/2H)MoS_(2)(P‐BMS)nanoflakes for hydrogen evolution reaction(HER).The doping of MoS_(2)with P atoms modifies its electronic structure and optimizes its electrocatalytic reaction kinetics,which significantly enhances its electrical conductivity and structural stability,which are verified by various characterization tools,including X‐ray photoelectron spectroscopy,high‐resolution transmission electron microscopy,X‐ray absorption near‐edge spectroscopy,and extended X‐ray absorption fine structure.Moreover,the hierarchically formed flakes of P‐BMS provide numerous catalytic surface‐active sites,which remarkably enhance its HER activity.The optimized P‐BMS electrocatalysts exhibit low overpotentials(60 and 72 mV at 10 mA cm^(−2))in H_(2)SO_(4)(0.5 M)and KOH(1.0 M),respectively.The mechanism of improving the HER activity of the material was systematically studied using density functional theory calculations and various electrochemical characterization techniques.This study has shown that phase engineering is a promising strategy for enhancing the H*adsorption of metal sulfides.
基金the National Key R&D Program of China(No.2022YFE0102000)the National Natural Science Foundation of China(Nos.22121004,U22A20409,22250008,and 22108197)+2 种基金the Haihe Laboratory of Sustainable Chemical Transformations,the Natural Science Foundation of Tianjin City(No.21JCZXJC00060)the Program of Introducing Talents of Discipline to Universities(No.BP0618007)the XPLORER PRIZE for financial support。
文摘The strategic manipulation of the interaction between a central metal atom and its coordinating environment in single-atom catalysts(SACs)is crucial for catalyzing the CO_(2)reduction reaction(CO_(2)RR).However,it remains a major challenge.While density-functional theory calculations serve as a powerful tool for catalyst screening,their time-consuming nature poses limitations.This paper presents a machine learning(ML)model based on easily accessible intrinsic descriptors to enable rapid,cost-effective,and high-throughput screening of efficient SACs in complex systems.Our ML model comprehensively captures the influences of interactions between 3 and 5d metal centers and 8 C,N-based coordination environments on CO_(2)RR activity and selectivity.We reveal the electronic origin of the different activity trends observed in early and late transition metals during coordination with N atoms.The extreme gradient boosting regression model shows optimal performance in predicting binding energy and limiting potential for both HCOOH and CO production.We confirm that the product of the electronegativity and the valence electron number of metals,the radius of metals,and the average electronegativity of neighboring coordination atoms are the critical intrinsic factors determining CO_(2)RR activity.Our developed ML models successfully predict several high-performance SACs beyond the existing database,demonstrating their potential applicability to other systems.This work provides insights into the low-cost and rational design of high-performance SACs.
基金supported by the National Natural Science Foundation of China(Grant nos.62090013,61974043,and 91833303)the National Key R&D Program of China(Grant no.2019YFB2203403)+1 种基金the Projects of Science and Technology Commission of Shanghai Municipality(Grant nos.21JC1402100 and 19511120100)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning.
文摘The practical application of Lithium-Sulfur batteries largely depends on highly efficient utilization and conversion of sulfur under the realistic condition of high-sulfur content and low electrolyte/sulfur ratio.Rational design of heterostructure electrocatalysts with abundant active sites and strong interfacial electronic interactions is a promising but still challenging strategy for preventing shuttling of polysulfides in lithium-sulfur batteries.Herein,ultrathin nonlayered NiO/Ni_(3)S_(2)heterostructure nanosheets are developed through topochemical transformation of layered Ni(OH)_(2)templates to improve the utilization of sulfur and facilitate stable cycling of batteries.As a multifunction catalyst,NiO/Ni_(3)S_(2)not only enhances the adsorption of polysulfides and shorten the transport path of Li ions and electrons but also promotes the Li_(2)S formation and transformation,which are verified by both in-situ Raman spectroscopy and electrochemical investigations.Thus,the cell with NiO/Ni_(3)S_(2)as electrocatalyst delivers an area capacity of 4.8 mAh cm^(-2)under the high sulfur loading(6 mg cm^(-2))and low electrolyte/sulfur ratio(4.3 pL mg^(-1)).The strategy can be extended to 2D Ni foil,demonstrating its prospects in the construction of electrodes with high gravimetric/volumetric energy densities.The designed electrocatalyst of ultrathin nonlayered heterostructure will shed light on achieving high energy density lithium-sulfur batteries.
基金supported by the Science and Technology Project of Sichuan Province(Grant No.2022YFS0447)the Local Science and Technology Development Fund Projects Guided by the Central Government of China(Grant No.2021ZYD0060)+2 种基金the Science and Technology Project of Southwest Petroleum University(Grant No.2021JBGS03)the Special Project of Science and Technology Strategic Cooperation between Nanchong City and Southwest Petroleum University(Grant No.SXQHJH064)the Postgraduate Research and Innovation Fund of Southwest Petroleum University(Grant No.2021CXYB14).
文摘Recently,metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications.The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory.Firstly,the catalytic activities of heterometallic clusters are investigated.Among all heterometallic clusters,Fe_(2)Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction,and Fe_(2)Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction,respectively 100 and 50 mV lower than those of Pt(111)and RuO_(2)(110)catalysts.The analysis of the potential gap of Fe_(2)M clusters indicates that Fe_(2)Mn,Fe_(2)Co,and Fe_(2)Ni clusters possess good bifunctional catalytic activity.Additionally,the catalytic activity of Fe_(2)Mn and Fe_(2)Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe_(2)M–PCN–Fe_(2)M is explored.Compared with Fe_(2)Mn–PCN–Fe_(2)Mn,Fe_(2)Co–PCN–Fe_(2)Co,and isolated Fe_(2)M clusters,the mixed-metal Fe_(2)Co–PCN–Fe_(2)Mn possesses excellent bifunctional catalytic activity,and the values of potential gap on the Mn and Co sites of Fe_(2)Co–PCN–Fe_(2)Mn are 0.69 and 0.70 V,respectively.Furthermore,the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst.In conclusion,the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.
基金financially supported by the National Natu-ral Science Foundation of China(Nos.52071024 and 52225103)the Project of International Cooperation and Exchanges NSFC(No.51961160729)+3 种基金the Funds for Creative Research Groups of China(No.51921001)the 111 Project(No.BP0719004)financial support from Projects of SKLAMM-USTB(No.2023-Z10)the Fundamental Research Fund for the Cen-tral Universities of China(No.FRF-TP-22-005C2).
文摘Self-supporting electrocatalysts for the oxygen evolution reaction(OER)require a delicate balance of cost-effectiveness,high activity,substantial durability,and robust mechanical properties.Here,we leverage the chemical and structural complexity of Al_(16.7) Fe_(16.7) Co_(16.7) Ni_(16.7) Cr_(16.7) Mn_(16.7)(at.%)high-entropy alloy(HEA)to address these requirements.Utilizing spinodal decomposition,we achieve a nanoporous structure of Fe-Cr-rich phase(A2 phase),providing a large specific surface area and robust mechanical integrity for free-standing applications.During cyclic voltammetry(CV)activation,an amorphous Mn-Fe-based HEA oxide forms in-situ on the nanoporous A2 phase,serving as an efficient electrocatalyst for OER in alkaline conditions.This nanoporous HEA amorphous oxide catalyst exhibits a low overpotential of 238 mV at a current density of 10 mA cm^(-2) and a low Tafel slope of 46 mV dec^(-1),surpassing the state-of-the-art RuO_(2) catalyst.This study establishes a competitive,engineering-applicable OER electrocatalyst and underscores the high-entropy effect’s potential in tuning electronic structures for enhanced performance.
基金supported by the National Natural Science Foundation of China(NSFCgrant no.22179065).
文摘Developing NO_(2)−reduction reaction(NO_(2)−RR)and oxygen evolution reaction(OER)bifunctional electrocatalysts at large current densities is crucial for decreasing energy consumption of electrocatalytic NH3 production and booming sustainable nitrogenbased economy.In addition to increasing active sites of catalysts,bubble adhesion deserves more attention during high-current electrolysis,which can deteriorate mass transfer and block active sites in gas-involving environments.Herein,super-hydrophilic/aerophobic cobalt-nickel-iron layered double hydroxide[Co(OH)_(2)/NiFe LDH]core-shell heterostructures were developed as efficient NO_(2)−RR and OER electrocatalysts to optimize surface tension due to self-pumping effect and modify active hydrogen adsorption behavior owing to moderate work function difference between Co(OH)_(2)and NiFe LDH.The fabricated Co(OH)_(2)/NiFe LDH exhibited excellent NO_(2)−RR activity(yield:50 mg h^(−1)cm^(−2);FE:91%at−500 mA cm^(−2))and impressive OER behavior(η1000:340 mV)accompanied by remarkable application potential for renewable energy-driven two-electrode system to produce NH3.This effort revealed important insights into the development of electrodes for reaching cost-effective electrocatalytic ammonia production at large current densities.
文摘Hydrogen generation and related energy applications heavily rely on the hydrogen evolution reaction(HER),which faces challenges of slow kinetics and high overpotential.Efficient electrocatalysts,particularly single-atom catalysts (SACs) on two-dimensional (2D) materials,are essential.This study presents a few-shot machine learning (ML) assisted high-throughput screening of 2D septuple-atomic-layer Ga_(2)CoS_(4-x)supported SACs to predict HER catalytic activity.Initially,density functional theory (DFT)calculations showed that 2D Ga_(2)CoS4is inactive for HER.However,defective Ga_(2)CoS_(4-x)(x=0–0.25)monolayers exhibit excellent HER activity due to surface sulfur vacancies (SVs),with predicted overpotentials (0–60 mV) comparable to or lower than commercial Pt/C,which typically exhibits an overpotential of around 50 m V in the acidic electrolyte,when the concentration of surface SV is lower than 8.3%.SVs generate spin-polarized states near the Fermi level,making them effective HER sites.We demonstrate ML-accelerated HER overpotential predictions for all transition metal SACs on 2D Ga_(2)CoS_(4-x).Using DFT data from 18 SACs,an ML model with high prediction accuracy and reduced computation time was developed.An intrinsic descriptor linking SAC atomic properties to HER overpotential was identified.This study thus provides a framework for screening SACs on 2D materials,enhancing catalyst design.
基金supported by the National Natural Science Foundation of China(21865025)the Program for Changjiang Scholars and Innovative Research Team in University(No.IRT_15R46)
文摘Defect engineering has been used to develop low-cost and effective catalysts to boost oxygen reduction reactions.However,the development of catalysts that use metal cation vacancies as the active sites for oxygen reduction reaction is lacking.In this study,ZnS nanoparticles on N-doped carbon serve as an oxygen reduction reaction catalyst.These catalysts were prepared via a one-step method at 900℃.Amazingly,the high-resolution transmission electron microscope image revealed obvious defects in the ZnS nanoparticles.These facilitated the catalyst synthesis,and the product displayed good electrocatalytic performance for the oxygen reduction reaction in an alkaline medium,including a lower onset potential,lower mid-wave potential,four electron transfer process,and better durability compared with 20 wt%Pt/C.More importantly,the density functional theory results indicated that using the Zn vacancies in the prepared catalyst as active sites required a lower reaction energy to produce OOH*from*OO toward oxygen reduction reaction.Therefore,the proposed catalyst with Zn vacancies can be used as a potential electrocatalyst and may be substitutes for Pt-based catalysts in fuel cells,given the novel catalyst’s resulting performance.
