沙特基础工业公司（SABIC）近日荣获2015年度责任关怀优异奖（Responsible Care Merit Award）,以表彰其在帮助关键利益相关方及所在社区实现可持续发展,并创造持续价值方面的卓越贡献.这是继2013年首次获奖后,SABIC在华第二度荣膺这一...沙特基础工业公司（SABIC）近日荣获2015年度责任关怀优异奖（Responsible Care Merit Award）,以表彰其在帮助关键利益相关方及所在社区实现可持续发展,并创造持续价值方面的卓越贡献.这是继2013年首次获奖后,SABIC在华第二度荣膺这一殊荣.展开更多
Triggering structural asymmetry can induce charge redistribution and modify electronic structures,which is of great significance for the design of high-performance hydrogen oxidation reaction(HOR)electrocatalysts.Here...Triggering structural asymmetry can induce charge redistribution and modify electronic structures,which is of great significance for the design of high-performance hydrogen oxidation reaction(HOR)electrocatalysts.Herein,we propose a dual anion-induced strategy to create an innovative RuS_(2)-RuO_(2)heterostructure featuring abundant S-Ru-O interfaces(RuS_(2)-RuO_(2)@C).This RuS_(2)-RuO_(2)@C demonstrates an impressive mass activity of 2.61 mAμg_(RU)^(-1)and an exchange current density of 2.96 mA cm^(-2),surpassing Pt/C and other comparative samples by over 20 times.Durability assessments confirm the superior stability of RuS_(2)-RuO_(2)@C,with only minimal performance loss during operation.Density functional theory(DFT)calculations indicate that the asymmetric S-Ru-O configuration optimizes the interfacial electronic structure and shifts the d-band center closer to the Fermi level,effectively reducing the energy barrier of the rate-determining step(RDS)in the alkaline HOR process.Moreover,in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)characteristics disclose the formation of a substantial hydrogen bond network at the S-Ru-o interface,which aids in the desorption of H_(2)O_(ad)and facilitates the vital Volmer step in the HOR pathway.展开更多
Amorphous bimetallic borides,as a new generation of catalytic nanomaterials with modifiable electronic properties,are of great importance in the design of high-efficiency catalysts for NaBH_(4) hydrolysis.This study s...Amorphous bimetallic borides,as a new generation of catalytic nanomaterials with modifiable electronic properties,are of great importance in the design of high-efficiency catalysts for NaBH_(4) hydrolysis.This study synthesizes an amorphous Co_(3)B-Mo_(2)B_(5) catalyst using a self-sacrificial template strategy and NaBH_(4) reduction for both NaBH_(4) hydrolysis and the reduction of 4-nitrophenol.The catalyst delivers an impressive hydrogen generation rate of 7690.5 mL min^(-1) g^(-1) at 25℃,coupled with a rapid reaction rate of 0.701 min^(-1) in the reduction of 4-nitrophenol.The enhanced catalytic performance is attributed to the unique amorphous structure and the electron rearrangement between Co_(3)B and Mo_(2)B_(5).Experimental and theoretical analyses suggest electron transfer from Co_(3)B to the Mo_(2)B_(5),with the electron-deficient Co_(3)B site favoring BH_(4)^(-) adsorption,while the electron-rich Mo_(2)B_(5) site favoring H_(2)O adsorption,Furthermore,Co_(3)B-Mo_(2)B_(5) demonstrated potential for energy applications,delivering a power output of 0.3 V in a hydrogen-air fuel cell.展开更多
Active and poisoning-resistant Ru-based electrocatalysts for the hydrogen oxidation reaction(HOR)are designed and fabricated by integrating Cu/Ru dual single atoms and alloy CuRu nanoparticles(N-(CuRu)_(NP+SA)@NC)thro...Active and poisoning-resistant Ru-based electrocatalysts for the hydrogen oxidation reaction(HOR)are designed and fabricated by integrating Cu/Ru dual single atoms and alloy CuRu nanoparticles(N-(CuRu)_(NP+SA)@NC)through a strategy involving weak chemical reduction and ammonia-assisted gas-phase nitridation.The resultant N-(CuRu)_(NP+SA)@NC electrocatalysts feature nitrogen atoms coordinated to both Cu and Ru metal atoms via strong N-metal interactions.Density functional theory calculations revealed that alloyed CuRu nanoparticles and monodispersed Cu atoms are vital for altering the electronic configuration of the host Ru elements.This finely tuned structure enhanced the adsorption of H and OH and promoted CO oxidation over the N-(CuRu)_(NP+SA)@NC electrocatalyst,resulting in high alkaline HOR activity,as evidenced by the higher exchange current density of 3.74 mA cm^(-2)and high mass activity of 3.28 mAμg_(Ru)^(-1),which are far superior to those of most Ru-based catalysts reported to date.Moreover,the N-(CuRu)_(NP+SA)@NC electrocatalysts are resistant to CO poisoning and can be used at a high concentration of 1000 ppm CO with no distinct decay in the activity,in stark contrast to the commercial Pt/C catalyst under the same conditions.展开更多
Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy ...Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.展开更多
Application of transition metal boride(TMB) catalysts towards hydrolysis of NaBH_(4) holds great significance to help relieve the energy crisis. Herein, we present a facile and versatile metal-organic framework(MOF) a...Application of transition metal boride(TMB) catalysts towards hydrolysis of NaBH_(4) holds great significance to help relieve the energy crisis. Herein, we present a facile and versatile metal-organic framework(MOF) assisted strategy to prepare Co_(2)B-CoPO_x with massive boron vacancies by introducing phytic acid(PA) cross-linked Co complexes that are acquired from reaction of PA and ZIF-67 into cobalt boride. The PA etching effectively breaks down the structure of ZIF-67 to create more vacancies, favoring the maximal exposure of active sites and elevation of catalytic activity. Experimental results demonstrate a drastic electronic interaction between Co and the dopant phosphorous(P), thereby the robustly electronegative P induces electron redistribution around the metal species, which facilitates the dissociation of B-H bond and the adsorption of H_(2)O molecules. The vacancy-rich Co_(2)B-CoPO_x catalyst exhibits scalable performance, characterized by a high hydrogen generation rate(HGR) of 7716.7 m L min^(-1)g^(-1) and a low activation energy(Ea) of 44.9 k J/mol, rivaling state-of-the-art catalysts. This work provides valuable insights for the development of advanced catalysts through P doping and boron vacancy engineering and the design of efficient and sustainable energy conversion systems.展开更多
Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR)...Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR).Herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).The disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of electrocatalyst.Consequently,Ru-RuS_(2)@C exhibits robust HOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),respectively.exceeding those of state-of-the-art Pt/C and most contemporary Ru-based HOR electrocatalysts.Surprisingly,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/C.Comprehensive analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of H and OH species,as well as lowers the energy barrier for water formation,thereby promoting theHoR performance.展开更多
Most advanced hydrogen evolution reaction(HER)catalysts show high activity under alkaline conditions.However,the performance deteriorates at a natural and acidic pH,which is often problematic in practical applications...Most advanced hydrogen evolution reaction(HER)catalysts show high activity under alkaline conditions.However,the performance deteriorates at a natural and acidic pH,which is often problematic in practical applications.Herein,a rhenium(Re)sulfide–transition-metal dichalcogenide heterojunc-tion catalyst with Re-rich vacancies(NiS_(2)-ReS_(2)-V)has been constructed.The optimized catalyst shows extraordinary electrocatalytic HER performance over a wide range of pH,with ultralow overpotentials of 42,85,and 122 mV under alkaline,acidic,and neutral conditions,respectively.Moreover,the two-electrode system with NiS_(2)-ReS_(2)-V1 as the cathode provides a voltage of 1.73 V at 500 mA cm^(-2),superior to industrial systems.Besides,the open-circuit voltage of a single Zn–H_(2)O cell with NiS_(2)-ReS_(2)-V1 as the cathode can reach an impressive 90.9% of the theoretical value,with a maximum power density of up to 31.6 mW cm^(-2).Moreover,it shows remarkable stability,with sustained discharge for approximately 120 h at 10 mA cm^(-2),significantly outperforming commercial Pt/C catalysts under the same conditions in all aspects.A series of systematic characterizations and theoretical calculations demonstrate that Re vacancies on the heterojunction interface would generate a stronger built-in electric field,which profoundly affects surface charge distribution and subsequently enhances HER performance.展开更多
Understanding and manipulating the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity.Herein,we present a synthesis of NiSe_(2)-Ce_(2)(CO_(3))_(2)O hetero...Understanding and manipulating the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity.Herein,we present a synthesis of NiSe_(2)-Ce_(2)(CO_(3))_(2)O heterostructure and demonstrate the efficacy of interfacial Ce_(2)(CO_(3))2O in promoting the formation of catalytically active centers to improve oxygen evolution activity.In-situ Raman spectroscopy shows that incorporation of Ce_(2)(CO_(3))2O into NiSe_(2) causes a cathodic shift of the Ni^(2+)→Ni~(3+) transition potential.Operando electrochemical impedance spectroscopy reveals that strong electronic coupling at heterogeneous interface accelerates charge transfer process.Furthermore,density functional theory calculations suggest that actual catalytic active species of NiOOH transformed from NiSe_(2),which is coupled with Ce_(2)(CO_(3))_(2)O,can optimize electronic structure and decrease the free energy barriers toward fast oxygen evolution reaction(OER) kinetics.Consequently,the resultant NiSe_(2)-Ce_(2)(CO_(3))_(2)O electrode exhibits remarkable electrocatalytic performance with low overpotentials(268/304 mV@50/100 mA cm^(-2)) and excellent stability(50 mA cm^(-2) for 120 h) in the alkaline electrolyte.This work emphasizes the significance of modulating the dynamic changes in developing efficient electrocatalyst.展开更多
基金supported by the National Natural Science Foundation of China(no.52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001,2018GXNSFAA294077)the Guangxi Technology Base and Talent Subject(GUIKE AD23023004,GUIKE AD20297039).
文摘Triggering structural asymmetry can induce charge redistribution and modify electronic structures,which is of great significance for the design of high-performance hydrogen oxidation reaction(HOR)electrocatalysts.Herein,we propose a dual anion-induced strategy to create an innovative RuS_(2)-RuO_(2)heterostructure featuring abundant S-Ru-O interfaces(RuS_(2)-RuO_(2)@C).This RuS_(2)-RuO_(2)@C demonstrates an impressive mass activity of 2.61 mAμg_(RU)^(-1)and an exchange current density of 2.96 mA cm^(-2),surpassing Pt/C and other comparative samples by over 20 times.Durability assessments confirm the superior stability of RuS_(2)-RuO_(2)@C,with only minimal performance loss during operation.Density functional theory(DFT)calculations indicate that the asymmetric S-Ru-O configuration optimizes the interfacial electronic structure and shifts the d-band center closer to the Fermi level,effectively reducing the energy barrier of the rate-determining step(RDS)in the alkaline HOR process.Moreover,in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)characteristics disclose the formation of a substantial hydrogen bond network at the S-Ru-o interface,which aids in the desorption of H_(2)O_(ad)and facilitates the vital Volmer step in the HOR pathway.
基金supported by the National Natural Science Foundation of China(Nos.52363028,21965005)Natural Science Foundation of Guangxi(Nos.2021GXNSFAA076001,2018GXNSFAA294077)Guangxi Technology Base and Talent Subject(Nos.GUIKE AD23023004,GUIKE AD20297039)。
文摘Amorphous bimetallic borides,as a new generation of catalytic nanomaterials with modifiable electronic properties,are of great importance in the design of high-efficiency catalysts for NaBH_(4) hydrolysis.This study synthesizes an amorphous Co_(3)B-Mo_(2)B_(5) catalyst using a self-sacrificial template strategy and NaBH_(4) reduction for both NaBH_(4) hydrolysis and the reduction of 4-nitrophenol.The catalyst delivers an impressive hydrogen generation rate of 7690.5 mL min^(-1) g^(-1) at 25℃,coupled with a rapid reaction rate of 0.701 min^(-1) in the reduction of 4-nitrophenol.The enhanced catalytic performance is attributed to the unique amorphous structure and the electron rearrangement between Co_(3)B and Mo_(2)B_(5).Experimental and theoretical analyses suggest electron transfer from Co_(3)B to the Mo_(2)B_(5),with the electron-deficient Co_(3)B site favoring BH_(4)^(-) adsorption,while the electron-rich Mo_(2)B_(5) site favoring H_(2)O adsorption,Furthermore,Co_(3)B-Mo_(2)B_(5) demonstrated potential for energy applications,delivering a power output of 0.3 V in a hydrogen-air fuel cell.
文摘Active and poisoning-resistant Ru-based electrocatalysts for the hydrogen oxidation reaction(HOR)are designed and fabricated by integrating Cu/Ru dual single atoms and alloy CuRu nanoparticles(N-(CuRu)_(NP+SA)@NC)through a strategy involving weak chemical reduction and ammonia-assisted gas-phase nitridation.The resultant N-(CuRu)_(NP+SA)@NC electrocatalysts feature nitrogen atoms coordinated to both Cu and Ru metal atoms via strong N-metal interactions.Density functional theory calculations revealed that alloyed CuRu nanoparticles and monodispersed Cu atoms are vital for altering the electronic configuration of the host Ru elements.This finely tuned structure enhanced the adsorption of H and OH and promoted CO oxidation over the N-(CuRu)_(NP+SA)@NC electrocatalyst,resulting in high alkaline HOR activity,as evidenced by the higher exchange current density of 3.74 mA cm^(-2)and high mass activity of 3.28 mAμg_(Ru)^(-1),which are far superior to those of most Ru-based catalysts reported to date.Moreover,the N-(CuRu)_(NP+SA)@NC electrocatalysts are resistant to CO poisoning and can be used at a high concentration of 1000 ppm CO with no distinct decay in the activity,in stark contrast to the commercial Pt/C catalyst under the same conditions.
基金supported by the National Natural Science Foundation of China(52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD18126001,GUIKE AD20297039)。
文摘Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.
基金supported by the National Natural Science Foundation of China (No.21965005)Natural Science Foundation of Guangxi Province (No.2021GXNSFAA076001)+1 种基金Guangxi Technology Base and Talent Subject (Nos.GUIKE AD18126001, GUIKE AD20297039)Innovation Project of Guangxi Graduate Education (Nos.YCSW2023140, YCBZ2023062)。
文摘Application of transition metal boride(TMB) catalysts towards hydrolysis of NaBH_(4) holds great significance to help relieve the energy crisis. Herein, we present a facile and versatile metal-organic framework(MOF) assisted strategy to prepare Co_(2)B-CoPO_x with massive boron vacancies by introducing phytic acid(PA) cross-linked Co complexes that are acquired from reaction of PA and ZIF-67 into cobalt boride. The PA etching effectively breaks down the structure of ZIF-67 to create more vacancies, favoring the maximal exposure of active sites and elevation of catalytic activity. Experimental results demonstrate a drastic electronic interaction between Co and the dopant phosphorous(P), thereby the robustly electronegative P induces electron redistribution around the metal species, which facilitates the dissociation of B-H bond and the adsorption of H_(2)O molecules. The vacancy-rich Co_(2)B-CoPO_x catalyst exhibits scalable performance, characterized by a high hydrogen generation rate(HGR) of 7716.7 m L min^(-1)g^(-1) and a low activation energy(Ea) of 44.9 k J/mol, rivaling state-of-the-art catalysts. This work provides valuable insights for the development of advanced catalysts through P doping and boron vacancy engineering and the design of efficient and sustainable energy conversion systems.
基金financially supported by the National Natural Science Foundation of China (52363028)the Natural Science Foundation of Guangxi Province (2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject (GUIKE AD23023004,GUIKE AD20297039)
文摘Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR).Herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).The disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of electrocatalyst.Consequently,Ru-RuS_(2)@C exhibits robust HOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),respectively.exceeding those of state-of-the-art Pt/C and most contemporary Ru-based HOR electrocatalysts.Surprisingly,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/C.Comprehensive analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of H and OH species,as well as lowers the energy barrier for water formation,thereby promoting theHoR performance.
基金This study was supported by the National Research Foundation of Korea(NRF-2021R1A2C4001777,NRF-2022M3H4A1A04096482 and RS-2023-00229679),the National Natural Science Foundation of China(No.21965005,52363028)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD20297039).
文摘Most advanced hydrogen evolution reaction(HER)catalysts show high activity under alkaline conditions.However,the performance deteriorates at a natural and acidic pH,which is often problematic in practical applications.Herein,a rhenium(Re)sulfide–transition-metal dichalcogenide heterojunc-tion catalyst with Re-rich vacancies(NiS_(2)-ReS_(2)-V)has been constructed.The optimized catalyst shows extraordinary electrocatalytic HER performance over a wide range of pH,with ultralow overpotentials of 42,85,and 122 mV under alkaline,acidic,and neutral conditions,respectively.Moreover,the two-electrode system with NiS_(2)-ReS_(2)-V1 as the cathode provides a voltage of 1.73 V at 500 mA cm^(-2),superior to industrial systems.Besides,the open-circuit voltage of a single Zn–H_(2)O cell with NiS_(2)-ReS_(2)-V1 as the cathode can reach an impressive 90.9% of the theoretical value,with a maximum power density of up to 31.6 mW cm^(-2).Moreover,it shows remarkable stability,with sustained discharge for approximately 120 h at 10 mA cm^(-2),significantly outperforming commercial Pt/C catalysts under the same conditions in all aspects.A series of systematic characterizations and theoretical calculations demonstrate that Re vacancies on the heterojunction interface would generate a stronger built-in electric field,which profoundly affects surface charge distribution and subsequently enhances HER performance.
基金financially National Natural Science Foundation of China (52363028, 21965005)Volkswagen Foundation (Freigeist Fellowship 89592)+2 种基金Natural Science Foundation of Guangxi Province (2021GXNSFAA076001)Guangxi Technology Base and Talent Subject (GUIKE AD23023004, GUIKE AD20297039)Innovation Project of Guangxi Graduate Education (Nos. YCSW2024219, YCBZ2024082)。
文摘Understanding and manipulating the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity.Herein,we present a synthesis of NiSe_(2)-Ce_(2)(CO_(3))_(2)O heterostructure and demonstrate the efficacy of interfacial Ce_(2)(CO_(3))2O in promoting the formation of catalytically active centers to improve oxygen evolution activity.In-situ Raman spectroscopy shows that incorporation of Ce_(2)(CO_(3))2O into NiSe_(2) causes a cathodic shift of the Ni^(2+)→Ni~(3+) transition potential.Operando electrochemical impedance spectroscopy reveals that strong electronic coupling at heterogeneous interface accelerates charge transfer process.Furthermore,density functional theory calculations suggest that actual catalytic active species of NiOOH transformed from NiSe_(2),which is coupled with Ce_(2)(CO_(3))_(2)O,can optimize electronic structure and decrease the free energy barriers toward fast oxygen evolution reaction(OER) kinetics.Consequently,the resultant NiSe_(2)-Ce_(2)(CO_(3))_(2)O electrode exhibits remarkable electrocatalytic performance with low overpotentials(268/304 mV@50/100 mA cm^(-2)) and excellent stability(50 mA cm^(-2) for 120 h) in the alkaline electrolyte.This work emphasizes the significance of modulating the dynamic changes in developing efficient electrocatalyst.
