Accelerated Hydrogen Evolution Kinetics on NiFe‐Layered Double Hydroxide Electrocatalysts by Tailoring Water Dissociation Active Sites

Owing to its earth abundance, low kinetic overpotential, and superior stability, NiFe‐layered double hydroxide (NiFe‐LDH) has emerged as a promising electrocatalyst for catalyzing water splitting, especially oxygen evolution reaction (OER), in alkaline solutions. Unfortunately, as a result of extremely sluggish water dissociation kinetics (Volmer step), hydrogen evolution reaction (HER) activity of the NiFe‐LDH is rather poor in alkaline environment. Here a novel strategy is demonstrated for substantially accelerating the hydrogen evolution kinetics of the NiFe‐LDH by partially substituting Fe atoms with Ru. In a 1 m KOH solution, the as‐synthesized Ru‐doped NiFe‐LDH nanosheets (NiFeRu‐LDH) exhibit excellent HER performance with an overpotential of 29 mV at 10 mA cm−2, which is much lower than those of noble metal Pt/C and reported electrocatalysts. Both experimental and theoretical results reveal that the introduction of Ru atoms into NiFe‐LDH can efficiently reduce energy barrier of the Volmer step, eventually accelerating its HER kinetics. Benefitting from its outstanding HER activity and remained excellent OER activity, the NiFeRu‐LDH steadily drives an alkaline electrolyzer with a current density of 10 mA cm−2 at a cell voltage of 1.52 V, which is much lower than the values for Pt/C–Ir/C couple and state‐of‐the‐art overall water‐splitting electrocatalysts.

[1]  Hong Liang,et al.  Enhancing Electrocatalytic Total Water Splitting at Few Layer Pt-NiFe Layered Double Hydroxide Interfaces , 2017 .

[2]  F. Gao,et al.  Electronic and Morphological Dual Modulation of Cobalt Carbonate Hydroxides by Mn Doping toward Highly Efficient and Stable Bifunctional Electrocatalysts for Overall Water Splitting. , 2017, Journal of the American Chemical Society.

[3]  S. Qiao,et al.  Design Strategies toward Advanced MOF‐Derived Electrocatalysts for Energy‐Conversion Reactions , 2017 .

[4]  Sheng Chen,et al.  Ultrathin metal-organic framework array for efficient electrocatalytic water splitting , 2017, Nature Communications.

[5]  Xiaodong Zhuang,et al.  Efficient hydrogen production on MoNi4 electrocatalysts with fast water dissociation kinetics , 2017, Nature Communications.

[6]  Qianwang Chen,et al.  Ruthenium-cobalt nanoalloys encapsulated in nitrogen-doped graphene as active electrocatalysts for producing hydrogen in alkaline media , 2017, Nature Communications.

[7]  Xiangwei Zhu,et al.  Ternary NiCo2Px Nanowires as pH‐Universal Electrocatalysts for Highly Efficient Hydrogen Evolution Reaction , 2017, Advanced materials.

[8]  Colin F. Dickens,et al.  Combining theory and experiment in electrocatalysis: Insights into materials design , 2017, Science.

[9]  Mark D. Symes,et al.  Earth-abundant catalysts for electrochemical and photoelectrochemical water splitting , 2017 .

[10]  Harry B Gray,et al.  Earth-Abundant Heterogeneous Water Oxidation Catalysts. , 2016, Chemical reviews.

[11]  Xiaodong Zhuang,et al.  Engineering water dissociation sites in MoS2 nanosheets for accelerated electrocatalytic hydrogen production , 2016 .

[12]  Xiaodong Zhuang,et al.  Interface Engineering of MoS2 /Ni3 S2 Heterostructures for Highly Enhanced Electrochemical Overall-Water-Splitting Activity. , 2016, Angewandte Chemie.

[13]  Zhiyi Lu,et al.  High-Performance Water Electrolysis System with Double Nanostructured Superaerophobic Electrodes. , 2016, Small.

[14]  S. E. Hosseini,et al.  Hydrogen production from renewable and sustainable energy resources: Promising green energy carrier for clean development , 2016 .

[15]  Z. Dai,et al.  Coupled molybdenum carbide and reduced graphene oxide electrocatalysts for efficient hydrogen evolution , 2016, Nature Communications.

[16]  M. Kanatzidis,et al.  Design of active and stable Co-Mo-Sx chalcogels as pH-universal catalysts for the hydrogen evolution reaction. , 2016, Nature materials.

[17]  Hung-Chih Chang,et al.  Efficient hydrogen evolution catalysis using ternary pyrite-type cobalt phosphosulphide. , 2015, Nature materials.

[18]  Wei Xing,et al.  NiSe Nanowire Film Supported on Nickel Foam: An Efficient and Stable 3D Bifunctional Electrode for Full Water Splitting. , 2015, Angewandte Chemie.

[19]  Xiaoxin Zou,et al.  Noble metal-free hydrogen evolution catalysts for water splitting. , 2015, Chemical Society reviews.

[20]  Xunyu Lu,et al.  Electrodeposition of hierarchically structured three-dimensional nickel–iron electrodes for efficient oxygen evolution at high current densities , 2015, Nature Communications.

[21]  X. Lou,et al.  Porous molybdenum carbide nano-octahedrons synthesized via confined carburization in metal-organic frameworks for efficient hydrogen production , 2015, Nature Communications.

[22]  Edward Ghali,et al.  Electrocatalysis developments for hydrogen evolution reaction in alkaline solutions – A Review , 2015 .

[23]  Min Wei,et al.  Layered double hydroxide-based nanomaterials as highly efficient catalysts and adsorbents. , 2014, Small.

[24]  Mohammad Khaja Nazeeruddin,et al.  Water photolysis at 12.3% efficiency via perovskite photovoltaics and Earth-abundant catalysts , 2014, Science.

[25]  David G. Evans,et al.  Catalytic applications of layered double hydroxides: recent advances and perspectives. , 2014, Chemical Society reviews.

[26]  Yongfeng Hu,et al.  Nanoscale nickel oxide/nickel heterostructures for active hydrogen evolution electrocatalysis , 2014, Nature Communications.

[27]  Qiu Yang,et al.  Three-dimensional NiFe layered double hydroxide film for high-efficiency oxygen evolution reaction. , 2014, Chemical communications.

[28]  Tom Regier,et al.  An advanced Ni-Fe layered double hydroxide electrocatalyst for water oxidation. , 2013, Journal of the American Chemical Society.

[29]  Maria Chan,et al.  Trends in activity for the water electrolyser reactions on 3d M(Ni,Co,Fe,Mn) hydr(oxy)oxide catalysts. , 2012, Nature materials.

[30]  Dermot O'Hare,et al.  Recent advances in the synthesis and application of layered double hydroxide (LDH) nanosheets. , 2012, Chemical reviews.

[31]  J. Goodenough,et al.  A Perovskite Oxide Optimized for Oxygen Evolution Catalysis from Molecular Orbital Principles , 2011, Science.

[32]  V. Stamenkovic,et al.  Enhancing Hydrogen Evolution Activity in Water Splitting by Tailoring Li+-Ni(OH)2-Pt Interfaces , 2011, Science.

[33]  James R. McKone,et al.  Solar water splitting cells. , 2010, Chemical reviews.

[34]  Dongke Zhang,et al.  Recent progress in alkaline water electrolysis for hydrogen production and applications , 2010 .

[35]  Y. Geletii,et al.  A Fast Soluble Carbon-Free Molecular Water Oxidation Catalyst Based on Abundant Metals , 2010, Science.

[36]  J. Nørskov,et al.  Computational high-throughput screening of electrocatalytic materials for hydrogen evolution , 2006, Nature materials.

[37]  John A. Turner,et al.  Sustainable Hydrogen Production , 2004, Science.

[38]  Abdullah M. Asiri,et al.  Recent Progress in Cobalt‐Based Heterogeneous Catalysts for Electrochemical Water Splitting , 2016, Advanced materials.