Oxygen evolution reaction （OER） electrolysis, as an important reaction involved in water splitting and rechargeable metal-air batteries, has attracted increasing attention for clean energy generation and efficient e...Oxygen evolution reaction （OER） electrolysis, as an important reaction involved in water splitting and rechargeable metal-air batteries, has attracted increasing attention for clean energy generation and efficient energy storage. Nickel/iron （NiFe）-based compounds have been known as active OER catalysts since the last century, and renewed interest has been witnessed in recent years on developing advanced NiFe-based materials for better activity and stability. In this review, we present the early discovery and recent progress on NiFe-based OER electrocatalysts in terms of chemical properties, synthetic methodologies and catalytic performances. The advantages and disadvantages of each class of NiFe-based compounds are summarized, including NiFe alloys, electrodeposited films and layered double hydroxide nanoplates. Some mechanistic studies of the active phase of NiFe-based compounds are introduced and discussed to give insight into the nature of active catalytic sites, which could facilitate further improving NiFe based OER electrocatalysts. Finally, some applications of NiFe- based compounds for OER are described, including the development of an electrolyzer operating with a single AAA battery with voltage below 1.5 V and high performance rechargeable Zn-air batteries.展开更多
Nanostructured materials have received tremendous interest due to their unique mechanical/electrical properties and overall behavior contributed by the complex synergy of bulk and interfacial properties for efficient ...Nanostructured materials have received tremendous interest due to their unique mechanical/electrical properties and overall behavior contributed by the complex synergy of bulk and interfacial properties for efficient and effective energy conversion and storage. The booming development of nanotechnology affords emerging but effective tools in designing advanced energy material. We reviewed the significant progress and dominated nanostructured energy materials in electrochemical energy conversion and storage devices, including lithium ion batteries, lithium-sulfur batteries, lithium-oxygen batteries, lithium metal batteries, and supercapacitors. The use of nanostructured electrocatalyst for effective electrocatalysis in oxygen reduction and oxygen evolution reactions for fuel cells and metal-air batteries was also included. The challenges in the undesirable side reactions between electrolytes and electrode due to high electrode/electrolyte contact area, low volumetric energy density of electrode owing to low tap density, and uniform production of complex energy materials in working devices should be overcome to fully demonstrate the advanced energy nanostructures for electrochemical energy conversion and storage. The energy chemistry at the interfaces of nanostructured electrode/electrolyte is highly expected to guide the rational design and full demonstration of energy materials in a working device. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.展开更多
A cost-efficient and stable oxygen evolution electrocatalyst is essential for improving energy storage and conversion efficiencies. Herein, 2D nanosheets with randomly cross-linked CoNi layered double hydroxide （LDH...A cost-efficient and stable oxygen evolution electrocatalyst is essential for improving energy storage and conversion efficiencies. Herein, 2D nanosheets with randomly cross-linked CoNi layered double hydroxide （LDH） and small CoO nanocrystals were designed and synthesized via in situ reduction and interface- directed assembly in air. The formation of CoNi LDH/CoO nanosheets was attributed to the strong extrusion of hydrated metal-oxide clusters driven by the interfacial tension. The obtained loose and porous nanosheets exhibited low crystallinity due to the presence of numerous defects. Owing to the orbital hybridization between metal 3d and O 2p orbitals, and electron transfer between metal atoms through Ni-O-Co, a number of Co and Ni atoms in the CoNi LDH present a high ＋3 valency. These unique characteristics result in a high density of oxygen evolution reaction （OER） active sites, improving the affinity between OH- and catalyst, and resulting in a large accessible surface area and permeable channels for ion adsorption and transport. Therefore, the resulting nanosheets exhibited high catalytic activity towards the OER. The CoNi LDH/CoO featured a low onset potential of 1.48 V in alkaline medium, and required an overpotential of only 300 mV at a current density of 10 mA.cm-2, while displaying good stability in accelerated durability tests.展开更多
Oxygen evolution reaction(OER),as an important half‐reaction involved in water splitting,has been intensely studied since the last century.Transition metal phosphide and sulfide‐based compounds have attracted increa...Oxygen evolution reaction(OER),as an important half‐reaction involved in water splitting,has been intensely studied since the last century.Transition metal phosphide and sulfide‐based compounds have attracted increasing attention as active OER catalysts due to their excellent physical and chemical characters,and massive efforts have been devoted to improving the phosphide and sulfide‐based materials with better activity and stability in recent years.In this review,the recent progress on phosphide and sulfide‐based OER electrocatalysts in terms of chemical properties,synthetic methodologies,catalytic performances evaluation and improvement strategy is reviewed.The most accepted reaction pathways as well as the thermodynamics and electrochemistry of the OER are firstly introduced in brief,followed by a summary of the recent research and optimization strategy of phosphide and sulfide‐based OER electrocatalysts.Finally,some mechanistic studies of the active phase of phosphide and sulfide‐based compounds are discussed to give insight into the nature of active catalytic sites.It is expected to indicate guidance for further improving the performances of phosphide and sulfide‐based OER electrocatalysts.展开更多
The development of high-efficiency electrocatalysts for oxygen evolution reactions （OERs） plays an important role in the water-splitting process. Herein, we report a facile way to obtain two-dimensional （2D） singl...The development of high-efficiency electrocatalysts for oxygen evolution reactions （OERs） plays an important role in the water-splitting process. Herein, we report a facile way to obtain two-dimensional （2D） single-unit-cell-thick layered double hydroxide （LDH） nanosheets （NSs, - 1.3 nm） within only 5 min. These nanosheets presented significantly enhanced OER performance compared to bulk LDH systems fabricated using the conventional co-precipitation method. The current strategy further allowed control over the chemical compositions and electrochemical activities of the LDH NSs. For example, CoFe-LDH NSs presented the lowest overpotential of 0.28 V at 10 mA/cm2, and the NiFe-LDHs NSs showed Tafel slopes of 33.4 mV/decade and nearly 100% faradaic efficiency, thus outperforming state-of-the-art IrO2 water electrolysis catalysts. Moreover, positron annihilation lifetime spectroscopy and high-resolution transmission electron microscopy observations confirmed that rich defects and distorted lattices occurred within the 2D LDH NSs, which could supply abundant electrochemically active OER sites. Periodic calculations based on density functional theory （DFT） further showed that the CoFe- and NiFe-LDHs presented very low energy gaps and obvious spin-polarization behavior, which facilitated high electron mobility during the OER process. Therefore, this work presents a combined experimental and theoretical study on 2D single-unit-cell-thick LDH NSs with high OER activities, which have potential application in water splitting for renewable energy.展开更多
The overall water splitting for hydrogen production is an effective strategy to resolve the environmental and energy crisis. Here, we report a facile approach to synthesize the Ir-based multimetallic, hierarchical, do...The overall water splitting for hydrogen production is an effective strategy to resolve the environmental and energy crisis. Here, we report a facile approach to synthesize the Ir-based multimetallic, hierarchical, double-coreshelled architecture(HCSA) assisted by oil bath reaction for boosting overall water splitting in acidic environment. The Ir Ni Cu HCSA shows superior electrocatalytic activity for hydrogen evolution reaction(HER) and oxygen evolution reaction(OER), which are comparable to commercial Pt/C and better than IrO2. The Ir Ni Cu HCSA exhibits remarkably catalytic efficiency as bifunctional catalyst for overall water splitting where a low cell voltage of 1.53 V is enough to drive a current density of 10 mA cm^-2 and maintains stable for at least 20 h. The presented work for the design and synthesis of novel Ir-based multimetallic architecture paves the way for highperformance overall water splitting catalysis.展开更多
Rational design and controllable synthesis of efficient electrocatalysts for water oxidation is of significant importance for the development of promising energy conversion systems, in particular integrated photoelect...Rational design and controllable synthesis of efficient electrocatalysts for water oxidation is of significant importance for the development of promising energy conversion systems, in particular integrated photoelectrochemical water splitting devices. Cobalt oxide(Co3O4) nanostructures with mixed valences(Ⅱ,Ⅲ)have been regarded as promising electrocatalysts for the oxygen evolution reaction(OER). They are able to promote catalytic support of OER but with only modest activity. Here, we demonstrate that the OER performance of cubic Co3O4 electrocatalyst is obviously improved when they are anchored on delaminated two-dimensional(2D) Ti3C2 MXene nanosheets. Upon activation the overpotential of the hybrid catalyst delivers 300 m V at a current density of 10 m A cm(2) in basic solutions, which is remarkably lower than those of Ti3C2 MXene and Co3O4 nanocubes. The strong interfacial electrostatic interactions between two components contribute to the exceptional catalytic performance and stability. The enhanced OER activity and facile synthesis make these Co3O4 nanocubes-decorated ultrathin 2D Ti3C2 MXene nanosheets useful for constructing efficient and stable electrodes for high-performance electrochemical water splitting.展开更多
Developing efficient water-splitting electrocatalysts, particularly for the anodic oxygen evolution reaction （OER）, is an important challenge in energy conversion technologies. In this study, we report the developme...Developing efficient water-splitting electrocatalysts, particularly for the anodic oxygen evolution reaction （OER）, is an important challenge in energy conversion technologies. In this study, we report the development of iron-doped nickel disulfide nanoarray on Ti mesh （Fe0.1-NiS2 NA/Ti） via the sulfidation of its nickel-iron-layered double hydroxide precursor （NiFe-LDH NAFFi）. As a three-dimensional OER anode, Fe0.1NiS2 NA/Ti exhibits remarkable activity and stability in 1.0 M KOH, with the requirement of a low overpotential of 231 mV to achieve 100 mA·cm^-2. In addition, it exhibits excellent activity and durability in 30 wt.% KOH. Notably, this electrode is also efficient for the cathodic hydrogen evolution reaction under alkaline conditions.展开更多
Hetero-structure induced high performance catalyst for oxygen evolution reaction(OER)in the water splitting reaction has received increased attention.Herein,we demonstrated a novel catalyst system of NiSe_(2)-CoSe_(2)...Hetero-structure induced high performance catalyst for oxygen evolution reaction(OER)in the water splitting reaction has received increased attention.Herein,we demonstrated a novel catalyst system of NiSe_(2)-CoSe_(2) consisting of nanorods and nanoparticles for the efficient OER in the alkaline electrolyte.This catalyst system can be easily fabricated via a low-temperature selenization of the solvothermal synthesized NiCo(OH)x precursor and the unique morphology of hybrid nanorods and nanoparticles was found by the electron microscopy analysis.The high valence state of the metal species was indicated by X-ray photoelectron spectroscopy study and a strong electronic effect was found in the NiSe_(2)-CoSe_(2) catalyst system compared to their counterparts.As a result,NiSe_(2)-CoSe_(2) exhibited high catalytic performance with a low overpotential of 250 mV to reach 10 mA·cm^(-2) for OER in the alkaline solution.Furthermore,high catalytic stability and catalytic kinetics were also observed.The superior performance can be attributed to the high valence states of Ni and Co and their strong synergetic coupling effect between the nanorods and nanoparticles,which could accelerate the charge transfer and offer abundant electrocatalytic active sites.The current work offers an efficient hetero-structure catalyst system for OER,and the results are helpful for the catalysis understanding.展开更多
Electrocatalysts with high catalytic activity and stability play a key role in promising renewable energy technologies, such as fuel cells and metal-air batteries. Here, we report the synthesis of Fe/Fe203 nanoparticl...Electrocatalysts with high catalytic activity and stability play a key role in promising renewable energy technologies, such as fuel cells and metal-air batteries. Here, we report the synthesis of Fe/Fe203 nanoparticles anchored on Fe-N-doped carbon nanosheets （Fe/Fe2Og@Fe-N-C） using shrimp shell-derived N-doped carbon nanodots as carbon and nitrogen sources in the presence of FeCI3 by a simple pyrolysis approach. Fe/Fe203@Fe-N-C obtained at a pyrolysis temperature of 1,000 ℃ （Fe/Fe2OB@Fe-N-C-1000） possessed a mesoporous structure and high surface area of 747.3 m2-g-1. As an electrocatalyst, Fe/Fe203@Fe-N-C-1000 exhibited bifunctional electrocatalytic activities toward the oxygen reduction reaction （ORR） and oxygen evolution reaction （OER） in alkaline media, com- parable to that of commercial Pt/C for ORR and RuO2 for OER, respectively. The Zn-air battery test demonstrated that Fe/Fe2OB@Fe-N-C-1000 had a superior rechargeable performance and cycling stability as an air cathode material with an open drcuit voltage of 1.47 V （vs. Ag/AgCl） and a power density of 193 mW.cm-2 at a current density of 220 mA-cm-2. These performances were better than other commercial catalysts with an open circuit voltage of 1.36 V and a power density of 173 mW-cm^-2 at a current density of 220 mA.cm-2 （a mixture of commercial Pt/C and RuO2 with a mass ratio of 1：1 was used for the rechargeable Zn-air battery measurements）. This work will be helpful to design and develop low-cost and abundant bifunctional oxygen electrocatalysts for future metal-air batteries.展开更多
Rational design and controlled fabrication of efficient and cost-effective electrodes for the oxygen evolution reaction （OER） are critical for addressing the unpre- cedented energy crisis. Nickel-iron layered double...Rational design and controlled fabrication of efficient and cost-effective electrodes for the oxygen evolution reaction （OER） are critical for addressing the unpre- cedented energy crisis. Nickel-iron layered double hydroxides （NiFe-LDHs） with specific interlayer anions （i.e. phosphate, phosphite, and hypophosphite） were fabricated by a co-predpitation method and investigated as oxygen evolution electrocatalysts. Intercalation of the phosphorus oxoanion enhanced the OER activity in an alkaline solution; the optimal performance （i.e., a low onset potential of 215 mV, a small Tafel slope of 37.7 mV/dec, and stable electrochemical behavior） was achieved with the hypophosphite-intercalated NiFe-LDH catalyst, demonstrating dramatic enhancement over the traditional carbonate-intercalated NiFe-LDH in terms of activity and durability. This enhanced performance is attributed to the interaction between the intercalated phosphorous oxoanions and the edge-sharing MO6 （M = Ni, Fe） layers, which modifies the surface electronic structure of the Ni sites. This concept should be inspiring for the design of more effective LDH-based oxygen evolution electrocatalvsts.展开更多
Oxygen evolution reaction(OER)is the core electrode reaction in energy-related technologies,such as electrolytic water,electrocatalytic carbon dioxide reduction,rechargeable metal-air batteries,and renewable fuel cell...Oxygen evolution reaction(OER)is the core electrode reaction in energy-related technologies,such as electrolytic water,electrocatalytic carbon dioxide reduction,rechargeable metal-air batteries,and renewable fuel cells.Development of well-stocked,cost-effective,and high-performance OER electrocatalysts is the key to the improvement of energy efficiency and the large-scale commercial implementation of these technologies.Multicomponent transition metal oxides and(oxy)hydroxides are the most promising OER catalysts due to their low cost,adjustable structure,high electrocatalytic activity,and outstanding durability.In this review,a brief overview about the mechanisms of OER is first offered,accompanied with the theory and calculation criteria.Then,the latest advances in the rational design of the related OER electrocatalysts and the modulation of the electronic structure of active sites are comprehensively summarized.Specifically,various strategies(including element doping,defect engineering,and fabrication of binderless catalysts)used to improve the OER performance are detailedly discussed,emphasizing the structure–function relationships.Finally,the challenges and perspectives on this promising field are proposed.展开更多
Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the ...Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the most conventional and classical non-noble metal-based electrocatalysts for OER,while TM basic salts[M^(2+)(OH)_(2-x)(A_(m^(-))_(x/m),A=CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)]consisting of OH−and another anion have drawn extensive research interest due to its higher catalytic activity in the past decade.In this review,we summarize the recent advances of TM basic salts and their application in OER and further overall water splitting.We categorize TM basic salt-based OER pre-catalysts into four types(CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)according to the anion,which is a key factor for their outstanding performance towards OER.We highlight experimental and theoretical methods for understanding the structure evolution during OER and the effect of anion on catalytic performance.To develop bifunctional TM basic salts as catalyst for the practical electrolysis application,we also review the present strategies for enhancing its hydrogen evolution reaction activity and thereby improving its overall water splitting performance.Finally,we conclude this review with a summary and perspective about the remaining challenges and future opportunities of TM basic salts as catalysts for water electrolysis.展开更多
文摘Oxygen evolution reaction （OER） electrolysis, as an important reaction involved in water splitting and rechargeable metal-air batteries, has attracted increasing attention for clean energy generation and efficient energy storage. Nickel/iron （NiFe）-based compounds have been known as active OER catalysts since the last century, and renewed interest has been witnessed in recent years on developing advanced NiFe-based materials for better activity and stability. In this review, we present the early discovery and recent progress on NiFe-based OER electrocatalysts in terms of chemical properties, synthetic methodologies and catalytic performances. The advantages and disadvantages of each class of NiFe-based compounds are summarized, including NiFe alloys, electrodeposited films and layered double hydroxide nanoplates. Some mechanistic studies of the active phase of NiFe-based compounds are introduced and discussed to give insight into the nature of active catalytic sites, which could facilitate further improving NiFe based OER electrocatalysts. Finally, some applications of NiFe- based compounds for OER are described, including the development of an electrolyzer operating with a single AAA battery with voltage below 1.5 V and high performance rechargeable Zn-air batteries.
基金supported by the National Key Research and Development Program (no.2016YFA0202500)National Basic Research Program of China (2015CB932500)the Natural Scientific Foundation of China (nos.21306102 and 21422604)
文摘Nanostructured materials have received tremendous interest due to their unique mechanical/electrical properties and overall behavior contributed by the complex synergy of bulk and interfacial properties for efficient and effective energy conversion and storage. The booming development of nanotechnology affords emerging but effective tools in designing advanced energy material. We reviewed the significant progress and dominated nanostructured energy materials in electrochemical energy conversion and storage devices, including lithium ion batteries, lithium-sulfur batteries, lithium-oxygen batteries, lithium metal batteries, and supercapacitors. The use of nanostructured electrocatalyst for effective electrocatalysis in oxygen reduction and oxygen evolution reactions for fuel cells and metal-air batteries was also included. The challenges in the undesirable side reactions between electrolytes and electrode due to high electrode/electrolyte contact area, low volumetric energy density of electrode owing to low tap density, and uniform production of complex energy materials in working devices should be overcome to fully demonstrate the advanced energy nanostructures for electrochemical energy conversion and storage. The energy chemistry at the interfaces of nanostructured electrode/electrolyte is highly expected to guide the rational design and full demonstration of energy materials in a working device. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
基金We gratefully acknowledge the support of this research by the Key Program Projects of the National Natural Science Foundation of China （No. 21031001）, the National Natural Science Foundation of China （Nos. 21371053 and 21573062）, the Cultivation Fund of the Key Scientific and Technical Innovation Project, Program for Innovative Research Team in University （No. IRT-1237）, Application Technology Research and Development Projects in Harbin （No. 2013AE4BW051）, International Science ＆ Technology Cooperation Program of China （No. 2014DFR41110）, and the Foundation of Heilongjiang Province of China （No. QC2013C009）.
文摘A cost-efficient and stable oxygen evolution electrocatalyst is essential for improving energy storage and conversion efficiencies. Herein, 2D nanosheets with randomly cross-linked CoNi layered double hydroxide （LDH） and small CoO nanocrystals were designed and synthesized via in situ reduction and interface- directed assembly in air. The formation of CoNi LDH/CoO nanosheets was attributed to the strong extrusion of hydrated metal-oxide clusters driven by the interfacial tension. The obtained loose and porous nanosheets exhibited low crystallinity due to the presence of numerous defects. Owing to the orbital hybridization between metal 3d and O 2p orbitals, and electron transfer between metal atoms through Ni-O-Co, a number of Co and Ni atoms in the CoNi LDH present a high ＋3 valency. These unique characteristics result in a high density of oxygen evolution reaction （OER） active sites, improving the affinity between OH- and catalyst, and resulting in a large accessible surface area and permeable channels for ion adsorption and transport. Therefore, the resulting nanosheets exhibited high catalytic activity towards the OER. The CoNi LDH/CoO featured a low onset potential of 1.48 V in alkaline medium, and required an overpotential of only 300 mV at a current density of 10 mA.cm-2, while displaying good stability in accelerated durability tests.
文摘Oxygen evolution reaction(OER),as an important half‐reaction involved in water splitting,has been intensely studied since the last century.Transition metal phosphide and sulfide‐based compounds have attracted increasing attention as active OER catalysts due to their excellent physical and chemical characters,and massive efforts have been devoted to improving the phosphide and sulfide‐based materials with better activity and stability in recent years.In this review,the recent progress on phosphide and sulfide‐based OER electrocatalysts in terms of chemical properties,synthetic methodologies,catalytic performances evaluation and improvement strategy is reviewed.The most accepted reaction pathways as well as the thermodynamics and electrochemistry of the OER are firstly introduced in brief,followed by a summary of the recent research and optimization strategy of phosphide and sulfide‐based OER electrocatalysts.Finally,some mechanistic studies of the active phase of phosphide and sulfide‐based compounds are discussed to give insight into the nature of active catalytic sites.It is expected to indicate guidance for further improving the performances of phosphide and sulfide‐based OER electrocatalysts.
基金This work was supported by the National Basic Research Program of China （No. 2014CB932103）, the National Natural Science Foundation of China （Nos. 21301016 and 21473013）, and the Beijing Municipal Natural Science Foundation （No. 2152016）.
文摘The development of high-efficiency electrocatalysts for oxygen evolution reactions （OERs） plays an important role in the water-splitting process. Herein, we report a facile way to obtain two-dimensional （2D） single-unit-cell-thick layered double hydroxide （LDH） nanosheets （NSs, - 1.3 nm） within only 5 min. These nanosheets presented significantly enhanced OER performance compared to bulk LDH systems fabricated using the conventional co-precipitation method. The current strategy further allowed control over the chemical compositions and electrochemical activities of the LDH NSs. For example, CoFe-LDH NSs presented the lowest overpotential of 0.28 V at 10 mA/cm2, and the NiFe-LDHs NSs showed Tafel slopes of 33.4 mV/decade and nearly 100% faradaic efficiency, thus outperforming state-of-the-art IrO2 water electrolysis catalysts. Moreover, positron annihilation lifetime spectroscopy and high-resolution transmission electron microscopy observations confirmed that rich defects and distorted lattices occurred within the 2D LDH NSs, which could supply abundant electrochemically active OER sites. Periodic calculations based on density functional theory （DFT） further showed that the CoFe- and NiFe-LDHs presented very low energy gaps and obvious spin-polarization behavior, which facilitated high electron mobility during the OER process. Therefore, this work presents a combined experimental and theoretical study on 2D single-unit-cell-thick LDH NSs with high OER activities, which have potential application in water splitting for renewable energy.
基金supported by the National Natural Science Foundation of China (51571151, 51701139, 51671143 and U1601216)
文摘The overall water splitting for hydrogen production is an effective strategy to resolve the environmental and energy crisis. Here, we report a facile approach to synthesize the Ir-based multimetallic, hierarchical, double-coreshelled architecture(HCSA) assisted by oil bath reaction for boosting overall water splitting in acidic environment. The Ir Ni Cu HCSA shows superior electrocatalytic activity for hydrogen evolution reaction(HER) and oxygen evolution reaction(OER), which are comparable to commercial Pt/C and better than IrO2. The Ir Ni Cu HCSA exhibits remarkably catalytic efficiency as bifunctional catalyst for overall water splitting where a low cell voltage of 1.53 V is enough to drive a current density of 10 mA cm^-2 and maintains stable for at least 20 h. The presented work for the design and synthesis of novel Ir-based multimetallic architecture paves the way for highperformance overall water splitting catalysis.
基金financial support from the National Natural Science Foundation of China (21975129, 51902164)Natural Science Foundation of Jiangsu Province (BK20180777, BK20190759)+4 种基金Natural Science Foundation of Jiangsu Higher Education Institutions of China (18KJB430018, 19KJB430003)Scientific Research Foundation for Advanced Talents (CXL2018046)Science Innovation Foundation for Young Scientists (CX2018012)supported by Student’s Platform for Innovation and Entrepreneurship Training Program in Jiangsu Province (201810298029Z)Student’s Platform for Innovation and Entrepreneurship Training Program (2018NFUSPITP602)。
文摘Rational design and controllable synthesis of efficient electrocatalysts for water oxidation is of significant importance for the development of promising energy conversion systems, in particular integrated photoelectrochemical water splitting devices. Cobalt oxide(Co3O4) nanostructures with mixed valences(Ⅱ,Ⅲ)have been regarded as promising electrocatalysts for the oxygen evolution reaction(OER). They are able to promote catalytic support of OER but with only modest activity. Here, we demonstrate that the OER performance of cubic Co3O4 electrocatalyst is obviously improved when they are anchored on delaminated two-dimensional(2D) Ti3C2 MXene nanosheets. Upon activation the overpotential of the hybrid catalyst delivers 300 m V at a current density of 10 m A cm(2) in basic solutions, which is remarkably lower than those of Ti3C2 MXene and Co3O4 nanocubes. The strong interfacial electrostatic interactions between two components contribute to the exceptional catalytic performance and stability. The enhanced OER activity and facile synthesis make these Co3O4 nanocubes-decorated ultrathin 2D Ti3C2 MXene nanosheets useful for constructing efficient and stable electrodes for high-performance electrochemical water splitting.
基金This work was supported by the National Natural Science Foundation of China （No. 21575137）.
文摘Developing efficient water-splitting electrocatalysts, particularly for the anodic oxygen evolution reaction （OER）, is an important challenge in energy conversion technologies. In this study, we report the development of iron-doped nickel disulfide nanoarray on Ti mesh （Fe0.1-NiS2 NA/Ti） via the sulfidation of its nickel-iron-layered double hydroxide precursor （NiFe-LDH NAFFi）. As a three-dimensional OER anode, Fe0.1NiS2 NA/Ti exhibits remarkable activity and stability in 1.0 M KOH, with the requirement of a low overpotential of 231 mV to achieve 100 mA·cm^-2. In addition, it exhibits excellent activity and durability in 30 wt.% KOH. Notably, this electrode is also efficient for the cathodic hydrogen evolution reaction under alkaline conditions.
基金The work is supported by the National Natural Science Foundation of China(21972124)the Priority Academic Program Development of Jiangsu Higher Education Institution.the support of the Six Talent Peaks Project of Jiangsu Province(XCL-070-2018)。
文摘Hetero-structure induced high performance catalyst for oxygen evolution reaction(OER)in the water splitting reaction has received increased attention.Herein,we demonstrated a novel catalyst system of NiSe_(2)-CoSe_(2) consisting of nanorods and nanoparticles for the efficient OER in the alkaline electrolyte.This catalyst system can be easily fabricated via a low-temperature selenization of the solvothermal synthesized NiCo(OH)x precursor and the unique morphology of hybrid nanorods and nanoparticles was found by the electron microscopy analysis.The high valence state of the metal species was indicated by X-ray photoelectron spectroscopy study and a strong electronic effect was found in the NiSe_(2)-CoSe_(2) catalyst system compared to their counterparts.As a result,NiSe_(2)-CoSe_(2) exhibited high catalytic performance with a low overpotential of 250 mV to reach 10 mA·cm^(-2) for OER in the alkaline solution.Furthermore,high catalytic stability and catalytic kinetics were also observed.The superior performance can be attributed to the high valence states of Ni and Co and their strong synergetic coupling effect between the nanorods and nanoparticles,which could accelerate the charge transfer and offer abundant electrocatalytic active sites.The current work offers an efficient hetero-structure catalyst system for OER,and the results are helpful for the catalysis understanding.
基金This work was financially supported by the National Natural Science Foundation of China （Nos. 51372248 and 51432009）, the Instrument Developing Project of the Chinese Academy of Sciences （No. yz201421） and the CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, the CAS Pioneer Hundred Talents Program and the Users with Potential Program （No. 2015HSC- UP006, Hefei Science Center, CAS）, China.
文摘Electrocatalysts with high catalytic activity and stability play a key role in promising renewable energy technologies, such as fuel cells and metal-air batteries. Here, we report the synthesis of Fe/Fe203 nanoparticles anchored on Fe-N-doped carbon nanosheets （Fe/Fe2Og@Fe-N-C） using shrimp shell-derived N-doped carbon nanodots as carbon and nitrogen sources in the presence of FeCI3 by a simple pyrolysis approach. Fe/Fe203@Fe-N-C obtained at a pyrolysis temperature of 1,000 ℃ （Fe/Fe2OB@Fe-N-C-1000） possessed a mesoporous structure and high surface area of 747.3 m2-g-1. As an electrocatalyst, Fe/Fe203@Fe-N-C-1000 exhibited bifunctional electrocatalytic activities toward the oxygen reduction reaction （ORR） and oxygen evolution reaction （OER） in alkaline media, com- parable to that of commercial Pt/C for ORR and RuO2 for OER, respectively. The Zn-air battery test demonstrated that Fe/Fe2OB@Fe-N-C-1000 had a superior rechargeable performance and cycling stability as an air cathode material with an open drcuit voltage of 1.47 V （vs. Ag/AgCl） and a power density of 193 mW.cm-2 at a current density of 220 mA-cm-2. These performances were better than other commercial catalysts with an open circuit voltage of 1.36 V and a power density of 173 mW-cm^-2 at a current density of 220 mA.cm-2 （a mixture of commercial Pt/C and RuO2 with a mass ratio of 1：1 was used for the rechargeable Zn-air battery measurements）. This work will be helpful to design and develop low-cost and abundant bifunctional oxygen electrocatalysts for future metal-air batteries.
文摘Rational design and controlled fabrication of efficient and cost-effective electrodes for the oxygen evolution reaction （OER） are critical for addressing the unpre- cedented energy crisis. Nickel-iron layered double hydroxides （NiFe-LDHs） with specific interlayer anions （i.e. phosphate, phosphite, and hypophosphite） were fabricated by a co-predpitation method and investigated as oxygen evolution electrocatalysts. Intercalation of the phosphorus oxoanion enhanced the OER activity in an alkaline solution; the optimal performance （i.e., a low onset potential of 215 mV, a small Tafel slope of 37.7 mV/dec, and stable electrochemical behavior） was achieved with the hypophosphite-intercalated NiFe-LDH catalyst, demonstrating dramatic enhancement over the traditional carbonate-intercalated NiFe-LDH in terms of activity and durability. This enhanced performance is attributed to the interaction between the intercalated phosphorous oxoanions and the edge-sharing MO6 （M = Ni, Fe） layers, which modifies the surface electronic structure of the Ni sites. This concept should be inspiring for the design of more effective LDH-based oxygen evolution electrocatalvsts.
基金supported by the National Natural Science Foundation of China(No.22075099)the Natural Science Foundation of Jilin Province(No.20220101051JC)the Education Department of Jilin Province(No.JJKH20220967KJ).
文摘Oxygen evolution reaction(OER)is the core electrode reaction in energy-related technologies,such as electrolytic water,electrocatalytic carbon dioxide reduction,rechargeable metal-air batteries,and renewable fuel cells.Development of well-stocked,cost-effective,and high-performance OER electrocatalysts is the key to the improvement of energy efficiency and the large-scale commercial implementation of these technologies.Multicomponent transition metal oxides and(oxy)hydroxides are the most promising OER catalysts due to their low cost,adjustable structure,high electrocatalytic activity,and outstanding durability.In this review,a brief overview about the mechanisms of OER is first offered,accompanied with the theory and calculation criteria.Then,the latest advances in the rational design of the related OER electrocatalysts and the modulation of the electronic structure of active sites are comprehensively summarized.Specifically,various strategies(including element doping,defect engineering,and fabrication of binderless catalysts)used to improve the OER performance are detailedly discussed,emphasizing the structure–function relationships.Finally,the challenges and perspectives on this promising field are proposed.
基金supported by the financial support from Natural Science Foundation of China(Nos.21871065,22209129 and 22071038)High-Level Innovation and Entrepreneurship(QCYRCXM-2022-123)+1 种基金support from the“Young Talent Support Plan”of Xi’an Jiaotong University(HG6J024)“Young Talent Lift Plan”of Xi’an city(095920221352).
文摘Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the most conventional and classical non-noble metal-based electrocatalysts for OER,while TM basic salts[M^(2+)(OH)_(2-x)(A_(m^(-))_(x/m),A=CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)]consisting of OH−and another anion have drawn extensive research interest due to its higher catalytic activity in the past decade.In this review,we summarize the recent advances of TM basic salts and their application in OER and further overall water splitting.We categorize TM basic salt-based OER pre-catalysts into four types(CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)according to the anion,which is a key factor for their outstanding performance towards OER.We highlight experimental and theoretical methods for understanding the structure evolution during OER and the effect of anion on catalytic performance.To develop bifunctional TM basic salts as catalyst for the practical electrolysis application,we also review the present strategies for enhancing its hydrogen evolution reaction activity and thereby improving its overall water splitting performance.Finally,we conclude this review with a summary and perspective about the remaining challenges and future opportunities of TM basic salts as catalysts for water electrolysis.
