Highly Stable Three-Dimensional Porous Nickel-Iron Nitride Nanosheets for Full Water Splitting at High Current Densities
TL;DR: P porous interconnected iron-nickel nitride nanosheets are designed and grown on carbon fiber cloth (FeNi-N/CFC); combining a facile electrodeposition method and in situ nitriding process to reveal its promising application in commercial electrolyzers.
Abstract: A noble-metal-free and highly efficient bifunctional catalyst for overall water splitting is greatly desirable to generate clean and sustainable energy carriers such as hydrogen, but enormous challenges remain. Herein, porous interconnected iron-nickel nitride nanosheets are designed and grown on carbon fiber cloth (FeNi-N/CFC); combining a facile electrodeposition method and in situ nitriding process. The as-synthesized FeNi-N/CFC, with a low mass loading of 0.25 mg cm-2 , exhibits excellent catalytic activities for both the oxygen evolution reaction (OER) with 20 mA cm-2 at an overpotential (η) of 232 mV and also the hydrogen evolution reaction (HER) with 10 mA cm-2 at η=106 mV. As a bifunctional electrocatalyst for overall water splitting FeNi-N/CFC only requires a cell voltage of 1.55 V to drive a current density (j) of 10 mA cm-2 and shows robust long-term durability at j>360 mA cm-2 with a negligible change in current density over 60 h; revealing its promising application in commercial electrolyzers.
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TL;DR: In this paper, a review of transition metal-based catalysts for the hydrogen evolution reaction (HER) is presented, and the challenges for the future development of novel catalysts are also analyzed.
Abstract: With the increasing demands in energy consumption and increasing environmental concerns, it is of vital significance for developing renewable and clean energy sources to substitute traditional fossil fuels. As an outstanding candidate, hydrogen is recognized as a green energy carrier due to its high gravimetric energy density, zero carbon footprints, and earth-abundance. Currently, water splitting in alkaline electrolytes represents one of the most promising methods for sustainable hydrogen production, and the key challenge lies in the development of high-performance electrocatalysts for the hydrogen evolution reaction (HER). Given the rapid advances in the design and development of efficient catalysts towards the alkaline HER, especially capable transition metal (TM)-based materials, this review aims to summarise recent progress in the theoretical understanding of the alkaline HER and TM-based electrocatalysts. TM-based catalysts classified by their different anionic compositions (metals, alloys, oxides, hydroxides, sulfides, selenides, tellurides, nitrides, phosphides, carbides, and borides) are comprehensively showcased. Special attention is given to mainstream strategies that can improve the catalytic properties of each category, as well as the underlying structure–activity regimes. Additionally, the challenges for the future development of novel catalysts are also analyzed.
418 citations
TL;DR: The most prominent theories are that the X-ides are either completely oxidized, left unoxidized, or transformed into core@shell particles upon testing as mentioned in this paper, but there is a lack of agreement regarding the composition of the true catalyst.
Abstract: Metal chalcogenides, pnictides, and carbides, labeled collectively as metal X-ides, have become an exciting new class of water oxidation electrocatalysts, but there is a lack of agreement regarding the composition of the “true” catalyst. The most prominent theories are that the X-ides are either completely oxidized, left unoxidized, or transformed into core@shell particles upon testing. Here, we examine examples of each conjecture, summarizing the conflicting viewpoints on catalyst identity and offering guidelines for more rigorous identification in the future. Most studies indicate that at least partial oxidation of the catalyst surface is critical to high performance, likely caused by an increased catalyst surface area upon oxidation or improved charge transfer in the X-ide cores. Therefore, more thorough and uniform long-term testing and nanoscale chemical analysis are essential to determine how these factors relate to catalyst performance.
267 citations
TL;DR: In this paper, transition metal nitrides (TMNs) have been used for electrochemical water splitting to produce high-purity hydrogen and oxygen as alternatives to fossil fuel.
Abstract: The hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) constitute the two main processes in electrochemical water splitting to produce high-purity hydrogen and oxygen as alternatives to fossil fuel. Catalysts are crucial to high-efficiency conversion of water to hydrogen and oxygen. Although transition metal nitrides (TMNs) are promising HER and OER catalysts due to the unique electronic structure and high electrical conductivity, single-phase nitrides have inferior activity compared to Pt-group metals because of the unsatisfactory metal–hydrogen (M–H) bonding strength. TMNs-based composites in combination with other metals, carbon materials, and metallic compounds have been demonstrated to possess improved catalytic properties because the modified electronic structure leads to balanced M–H bonding strength, synergistic effects, and improved electrochemical stability. Herein, recent progress pertaining to TMNs is reviewed from the perspective of advanced catalysts for electrochemical water splitting. The challenges and future opportunities confronting TMNs-based catalysts are also discussed.
256 citations
TL;DR: In this article, the ternary NiFeMoS anemones-like nanorods with scaly surface supported on nickel foam have been synthesized through a two-step method, where the NiFe hydroxides film has been electrodeposited on the surface of NF, leading to a homogeneous doping of NiFe.
201 citations
TL;DR: In this paper, a bamboo-structured nitrogen-doped carbon nanotube coencapped with metallic cobalt and Mo2C nanoparticles is designed and synthesized by a successive pyrolysis approach and demonstrated to be an efficient and stable bifunctional electrocatalyst for overall water splitting in alkaline medium.
Abstract: Developing efficient bifunctional electrocatalysts based on inexpensive and earth-abundant materials for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is essential for large-scale renewable energy storage and conversion processes but remains a major challenge. In this study, a bamboo-structured nitrogen-doped carbon nanotube coencapsulated with metallic cobalt and Mo2C nanoparticles (Co–Mo2C@NCNT) is designed and synthesized by a successive pyrolysis approach and demonstrated to be an efficient and stable bifunctional electrocatalyst for overall water splitting in alkaline medium. Attributing to favorable synergy interaction in composition and structure, the resultant Co–Mo2C@NCNT presents the superior performances toward HER, OER, and even overall water splitting in alkaline medium. To drive a current density of 10 mA cm–2, it needs only an overpotential of ∼186 and ∼377 mV for the electrocatalytic HER and OER, respectively, and a relatively low cell voltage (∼1.628 V) for overall...
142 citations
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TL;DR: The biggest challenge is whether or not the goals need to be met to fully utilize solar energy for the global energy demand can be met in a costeffective way on the terawatt scale.
Abstract: Energy harvested directly from sunlight offers a desirable approach toward fulfilling, with minimal environmental impact, the need for clean energy. Solar energy is a decentralized and inexhaustible natural resource, with the magnitude of the available solar power striking the earth’s surface at any one instant equal to 130 million 500 MW power plants.1 However, several important goals need to be met to fully utilize solar energy for the global energy demand. First, the means for solar energy conversion, storage, and distribution should be environmentally benign, i.e. protecting ecosystems instead of steadily weakening them. The next important goal is to provide a stable, constant energy flux. Due to the daily and seasonal variability in renewable energy sources such as sunlight, energy harvested from the sun needs to be efficiently converted into chemical fuel that can be stored, transported, and used upon demand. The biggest challenge is whether or not these goals can be met in a costeffective way on the terawatt scale.2
8,037 citations
TL;DR: The active site for hydrogen evolution, a reaction catalyzed by precious metals, on nanoparticulate molybdenum disulfide (MoS2) is determined by atomically resolving the surface of this catalyst before measuring electrochemical activity in solution.
Abstract: The identification of the active sites in heterogeneous catalysis requires a combination of surface sensitive methods and reactivity studies. We determined the active site for hydrogen evolution, a reaction catalyzed by precious metals, on nanoparticulate molybdenum disulfide (MoS2) by atomically resolving the surface of this catalyst before measuring electrochemical activity in solution. By preparing MoS2 nanoparticles of different sizes, we systematically varied the distribution of surface sites on MoS2 nanoparticles on Au(111), which we quantified with scanning tunneling microscopy. Electrocatalytic activity measurements for hydrogen evolution correlate linearly with the number of edge sites on the MoS2 catalyst.
4,930 citations
TL;DR: In this paper, the authors report a protocol for evaluating the activity, stability, and Faradaic efficiency of electrodeposited oxygen-evolving electrocatalysts for water oxidation.
Abstract: Objective evaluation of the activity of electrocatalysts for water oxidation is of fundamental importance for the development of promising energy conversion technologies including integrated solar water-splitting devices, water electrolyzers, and Li-air batteries. However, current methods employed to evaluate oxygen-evolving catalysts are not standardized, making it difficult to compare the activity and stability of these materials. We report a protocol for evaluating the activity, stability, and Faradaic efficiency of electrodeposited oxygen-evolving electrocatalysts. In particular, we focus on methods for determining electrochemically active surface area and measuring electrocatalytic activity and stability under conditions relevant to an integrated solar water-splitting device. Our primary figure of merit is the overpotential required to achieve a current density of 10 mA cm–2 per geometric area, approximately the current density expected for a 10% efficient solar-to-fuels conversion device. Utilizing ...
4,808 citations
TL;DR: This study shows that these r-RuO2 and r-IrO2 NPs can serve as a benchmark in the development of active OER catalysts for electrolyzers, metal-air batteries, and photoelectrochemical water splitting applications.
Abstract: The activities of the oxygen evolution reaction (OER) on iridium-oxide- and ruthenium-oxide-based catalysts are among the highest known to date. However, the OER activities of thermodynamically stable rutile iridium oxide (r-IrO2) and rutile iridium oxide (r-RuO2), normalized to catalyst mass or true surface area are not well-defined. Here we report a synthesis of r-IrO2 and r-RuO2 nanoparticles (NPs) of ∼6 nm, and examine their OER activities in acid and alkaline solutions. Both r-IrO2 and r-RuO2 NPs were highly active for OER, with r-RuO2 exhibiting up to 10 A/goxide at 1.48 V versus reversible hydrogen electrode. When comparing the two, r-RuO2 NPs were found to have slightly higher intrinsic and mass OER activities than r-IrO2 in both acid and basic solutions. Interestingly, these oxide NPs showed higher stability under OER conditions than commercial Ru/C and Ir/C catalysts. Our study shows that these r-RuO2 and r-IrO2 NPs can serve as a benchmark in the development of active OER catalysts for electrol...
2,762 citations
TL;DR: The Scope of Review: Large-Scale Centralized Energy Storage, Chemical Energy Storage: Solar Fuels, and Capacitors 6486 5.1.2.
Abstract: 1. Setting the Scope of the Challenge 6474 1.1. The Need for Solar Energy Supply and Storage 6474 1.2. An Imperative for Discovery Research 6477 1.3. Scope of Review 6478 2. Large-Scale Centralized Energy Storage 6478 2.1. Pumped Hydroelectric Energy Storage (PHES) 6479 2.2. Compressed Air Energy Storage (CAES) 6480 3. Smaller Scale Grid and Distributed Energy Storage 6481 3.1. Flywheel Energy Storage (FES) 6481 3.2. Superconducting Magnetic Energy Storage 6482 4. Chemical Energy Storage: Electrochemical 6482 4.1. Batteries 6482 4.1.1. Lead-Acid Batteries 6483 4.1.2. Alkaline Batteries 6484 4.1.3. Lithium-Ion Batteries 6484 4.1.4. High-Temperature Sodium Batteries 6484 4.1.5. Liquid Flow Batteries 6485 4.1.6. Metal-Air Batteries 6485 4.2. Capacitors 6485 5. Chemical Energy Storage: Solar Fuels 6486 5.1. Solar Fuels in Nature 6486 5.2. Artificial Photosynthesis and General Considerations of Water Splitting 6486
2,570 citations