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Title: Partially reduced Ru/RuO2 composites as efficient and pH-universal electrocatalysts for hydrogen evolution

Journal Article · · Energy & Environmental Science
DOI: https://doi.org/10.1039/d1ee02380b · OSTI ID:1838053

Efficient and long-term stable electrocatalysts for the hydrogen evolution reaction (HER) via water splitting are urgently desired to ease the energy crisis and develop the sustainability of human society. However, the HER performance of state-of-the-art Pt in non-acidic solutions is unsatisfactory due to the severely sluggish kinetics. In this work, DFT theoretical calculations reveal that the Ru/RuO2 composites enable high HER activity to be pursued under non-acidic conditions because of the distinctive Ru and RuO2 interface, which possess not only a strong capability to adsorb and dissociate water but also appropriate binding energies of H and OH. Therefore, we employ a simple strategy, including heating under an oxygen-poor environment and/or in situ electrochemical reduction, to partially reduce RuO2. The formed Ru/RuO2 interfaces demonstrate superior HER activities (e.g. η10 = 17 mV, 35 mV dec–1 in 1 M KOH) than Pt/C (e.g. η10 = 27 mV, 58 mV dec–1 in 1 M KOH) at both small (10–100 mA cm–2) and large (1 A cm–2) current densities in alkaline solution and even real seawater. Comprehensive experiments were conducted to investigate the structure-HER performance relationships. Moreover, benefiting from the bifunctional character of RuO2, a two-electrode system based on Ru/RuO2 composites and RuO2 exhibits the lowest cell voltage for water splitting in both 1 M KOH and 0.5 M H2SO4, respectively. A 300 h-stability test at 10 mA cm–2 without an obvious decay demonstrates the industrial prospects of the Ru/RuO2 composites to generate green energy.

Research Organization:
Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Natural Science Foundation of China (NSFC)
Grant/Contract Number:
FG02-86ER13622
OSTI ID:
1838053
Journal Information:
Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 10 Vol. 14; ISSN 1754-5692
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (58)

Hydrogen Evolution and Oxidation: Mechanistic Studies and Material Advances journal December 2018
Electrocatalysts for Hydrogen Evolution in Alkaline Electrolytes: Mechanisms, Challenges, and Prospective Solutions journal November 2017
Pseudomorphic Transformation of Interpenetrated Prussian Blue Analogs into Defective Nickel Iron Selenides for Enhanced Electrochemical and Photo-Electrochemical Water Splitting journal November 2018
Ruthenium‐Based Single‐Atom Alloy with High Electrocatalytic Activity for Hydrogen Evolution journal April 2019
Ni‐Activated Transition Metal Carbides for Efficient Hydrogen Evolution in Acidic and Alkaline Solutions journal August 2020
A General Route to Prepare Low‐Ruthenium‐Content Bimetallic Electrocatalysts for pH‐Universal Hydrogen Evolution Reaction by Using Carbon Quantum Dots journal January 2020
Metallic Ni3Mo3N Porous Microrods with Abundant Catalytic Sites as Efficient Electrocatalyst for Large Current Density and Superstability of Hydrogen Evolution Reaction and Water Splitting journal September 2020
Co-Fe-P nanotubes electrocatalysts derived from metal-organic frameworks for efficient hydrogen evolution reaction under wide pH range journal February 2019
Synthesis, Characterization, and Properties of Metal Phosphide Catalysts for the Hydrogen-Evolution Reaction journal August 2016
Structural Changes in RuO 2 during Electrochemical Hydrogen Evolution journal March 2016
In Situ Studies of the Electrochemical Reduction of a Supported Ultrathin Single-Crystalline RuO 2 (110) Layer in an Acidic Environment journal January 2019
Developments of Metal Phosphides as Efficient OER Precatalysts journal December 2016
Metal/Oxide Interface Nanostructures Generated by Surface Segregation for Electrocatalysis journal October 2015
Growth of One-Dimensional RuO 2 Nanowires on g-Carbon Nitride: An Active and Stable Bifunctional Electrocatalyst for Hydrogen and Oxygen Evolution Reactions at All pH Values journal October 2016
Nanoceria-Supported Ruthenium(0) Nanoparticles: Highly Active and Stable Catalysts for Hydrogen Evolution from Water journal February 2018
Constructing Bifunctional 3D Holey and Ultrathin CoP Nanosheets for Efficient Overall Water Splitting journal July 2019
Recent Trends and Perspectives in Electrochemical Water Splitting with an Emphasis on Sulfide, Selenide, and Phosphide Catalysts of Fe, Co, and Ni: A Review journal November 2016
Crystallinity Dependence of Ruthenium Nanocatalyst toward Hydrogen Evolution Reaction journal May 2018
In Situ Growth of Ni 2 P–Cu 3 P Bimetallic Phosphide with Bicontinuous Structure on Self-Supported NiCuC Substrate as an Efficient Hydrogen Evolution Reaction Electrocatalyst journal June 2019
The Role of Ru in Improving the Activity of Pd toward Hydrogen Evolution and Oxidation Reactions in Alkaline Solutions journal September 2019
Hydrogen Generation from Seawater Electrolysis over a Sandwich-like NiCoN|Ni x P|NiCoN Microsheet Array Catalyst journal July 2020
Metal–Organic Framework-Derived CoWP@C Composite Nanowire Electrocatalyst for Efficient Water Splitting journal May 2018
Solar Water Splitting Cells journal November 2010
Surface Chemistry of Ruthenium Dioxide in Heterogeneous Catalysis and Electrocatalysis: From Fundamental to Applied Research journal March 2012
Carbon Monoxide Hydrogenation on the Ru(001) Surface at Low Temperature Using Gas-Phase Atomic Hydrogen: Spectroscopic Evidence for the Carbonyl Insertion Mechanism on a Transition Metal Surface journal March 1995
Li x NiO/Ni Heterostructure with Strong Basic Lattice Oxygen Enables Electrocatalytic Hydrogen Evolution with Pt-like Activity journal February 2020
High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst journal December 2016
Formation of RuO(OH) 2 on RuO 2 -Based Electrodes for Hydrogen Production journal July 2014
Correction: Corrigendum: Ruthenium-cobalt nanoalloys encapsulated in nitrogen-doped graphene as active electrocatalysts for producing hydrogen in alkaline media journal June 2017
Interfacial water reorganization as a pH-dependent descriptor of the hydrogen evolution rate on platinum electrodes journal March 2017
Trends in activity for the water electrolyser reactions on 3d M(Ni,Co,Fe,Mn) hydr(oxy)oxide catalysts journal May 2012
An efficient and pH-universal ruthenium-based catalyst for the hydrogen evolution reaction journal February 2017
Ruthenium atomically dispersed in carbon outperforms platinum toward hydrogen evolution in alkaline media journal February 2019
Multi-site electrocatalysts for hydrogen evolution in neutral media by destabilization of water molecules journal December 2018
Single platinum atoms immobilized on an MXene as an efficient catalyst for the hydrogen evolution reaction journal December 2018
Engineering the electronic structure of single atom Ru sites via compressive strain boosts acidic water oxidation electrocatalysis journal March 2019
Nanostructured hydrotreating catalysts for electrochemical hydrogen evolution journal January 2014
An amorphous FeMoS 4 nanorod array toward efficient hydrogen evolution electrocatalysis under neutral conditions journal January 2017
Highly uniform Ru nanoparticles over N-doped carbon: pH and temperature-universal hydrogen release from water reduction journal January 2018
Boosting the hydrogen evolution performance of ruthenium clusters through synergistic coupling with cobalt phosphide journal January 2018
Ruthenium/nitrogen-doped carbon as an electrocatalyst for efficient hydrogen evolution in alkaline solution journal January 2017
Low-ruthenium-content NiRu nanoalloys encapsulated in nitrogen-doped carbon as highly efficient and pH-universal electrocatalysts for the hydrogen evolution reaction journal January 2018
Enhanced electrocatalytic performance for the hydrogen evolution reaction through surface enrichment of platinum nanoclusters alloying with ruthenium in situ embedded in carbon journal January 2018
Water splitting by electrolysis at high current densities under 1.6 volts journal January 2018
A sea-change: manganese doped nickel/nickel oxide electrocatalysts for hydrogen generation from seawater journal January 2018
Efficient alkaline hydrogen evolution on atomically dispersed Ni–N x Species anchored porous carbon with embedded Ni nanoparticles by accelerating water dissociation kinetics journal January 2019
Highly stable single Pt atomic sites anchored on aniline-stacked graphene for hydrogen evolution reaction journal January 2019
Trapping [PMo 12 O 40 ] 3− clusters into pre-synthesized ZIF-67 toward Mo x Co x C particles confined in uniform carbon polyhedrons for efficient overall water splitting journal January 2018
Multi-compositional hierarchical nanostructured Ni 3 S 2 @MoS x /NiO electrodes for enhanced electrocatalytic hydrogen generation and energy storage journal January 2018
A universal synthesis strategy for P-rich noble metal diphosphide-based electrocatalysts for the hydrogen evolution reaction journal January 2019
Seamlessly conductive Co(OH) 2 tailored atomically dispersed Pt electrocatalyst with a hierarchical nanostructure for an efficient hydrogen evolution reaction journal January 2020
Recent progress on nanostructured bimetallic electrocatalysts for water splitting and electroreduction of carbon dioxide journal September 2020
Ab initiomolecular dynamics for liquid metals journal January 1993
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Generalized Gradient Approximation Made Simple journal October 1996
Sustainable Hydrogen Production journal August 2004
Enhancing Hydrogen Evolution Activity in Water Splitting by Tailoring Li+-Ni(OH)2-Pt Interfaces journal December 2011
Combining theory and experiment in electrocatalysis: Insights into materials design journal January 2017