3D Self-Supported Fe-Doped Ni2P Nanosheet Arrays as Bifunctional Catalysts for Overall Water Splitting
TL;DR: In this paper, 3D self-supported Fe-doped Ni2P nanosheet arrays are synthesized on Ni foam by hydrothermal method followed by in situ phosphorization, which serve as bifunctional electrocatalysts for overall water splitting.
Abstract: The development of highly efficient bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is crucial for improving the efficiency of overall water splitting, but still remains challenging issue. Herein, 3D self-supported Fe-doped Ni2P nanosheet arrays are synthesized on Ni foam by hydrothermal method followed by in situ phosphorization, which serve as bifunctional electrocatalysts for overall water splitting. The as-synthesized (Ni0.33Fe0.67)2P with moderate Fe doping shows an outstanding OER performance, which only requires an overpotential of ≈230 mV to reach 50 mA cm−2 and is more efficient than the other Fe incorporated Ni2P electrodes. In addition, the (Ni0.33Fe0.67)2P exhibits excellent activity toward HER with a small overpotential of ≈214 mV to reach 50 mA cm−2. Furthermore, an alkaline electrolyzer is measured using (Ni0.33Fe0.67)2P electrodes as cathode and anode, respectively, which requires cell voltage of 1.49 V to reach 10 mA cm−2 as well as shows excellent stability with good nanoarray construction. Such good performance is attributed to the high intrinsic activity and superaerophobic surface property.
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TL;DR: A novel hybrid nanostructure with CoP nanoparticles embedded in a N-doped carbon nanotube hollow polyhedron (NCNHP) through a pyrolysis-oxidation-phosphidation strategy derived from core-shell ZIF-8@ZIF-67 is reported, benefiting from the synergistic effects between highly active CoP NPs and NCNHP.
Abstract: The construction of highly active and stable non-noble-metal electrocatalysts for hydrogen and oxygen evolution reactions is a major challenge for overall water splitting. Herein, we report a novel hybrid nanostructure with CoP nanoparticles (NPs) embedded in a N-doped carbon nanotube hollow polyhedron (NCNHP) through a pyrolysis–oxidation–phosphidation strategy derived from core–shell ZIF-8@ZIF-67. Benefiting from the synergistic effects between highly active CoP NPs and NCNHP, the CoP/NCNHP hybrid exhibited outstanding bifunctional electrocatalytic performances. When the CoP/NCNHP was employed as both the anode and cathode for overall water splitting, a potential as low as 1.64 V was needed to achieve the current density of 10 mA·cm–2, and it still exhibited superior activity after continuously working for 36 h with nearly negligible decay in potential. Density functional theory calculations indicated that the electron transfer from NCNHP to CoP could increase the electronic states of the Co d-orbital a...
1,411 citations
TL;DR: The fundamentals of HER are summarized and the recent state-of-the-art advances in the low-cost and high-performance catalysts based on noble and non-noble metals, as well as metal-free HER electrocatalysts are reviewed.
Abstract: Hydrogen fuel is considered as the cleanest renewable resource and the primary alternative to fossil fuels for future energy supply. Sustainable hydrogen generation is the major prerequisite to realize future hydrogen economy. The electrocatalytic hydrogen evolution reaction (HER), as the vital step of water electrolysis to H2 production, has been the subject of extensive study over the past decades. In this comprehensive review, we first summarize the fundamentals of HER and review the recent state-of-the-art advances in the low-cost and high-performance catalysts based on noble and non-noble metals, as well as metal-free HER electrocatalysts. We systemically discuss the insights into the relationship among the catalytic activity, morphology, structure, composition, and synthetic method. Strategies for developing an effective catalyst, including increasing the intrinsic activity of active sites and/or increasing the number of active sites, are summarized and highlighted. Finally, the challenges, perspectives, and research directions of HER electrocatalysis are featured.
1,387 citations
TL;DR: Focusing on self-supported electrodes, the latest advances in their structural design, controllable synthesis, mechanistic understanding, and strategies for performance enhancement are presented.
Abstract: Electrochemical water splitting is a promising technology for sustainable conversion, storage, and transport of hydrogen energy. Searching for earth-abundant hydrogen/oxygen evolution reaction (HER/OER) electrocatalysts with high activity and durability to replace noble-metal-based catalysts plays paramount importance in the scalable application of water electrolysis. A freestanding electrode architecture is highly attractive as compared to the conventional coated powdery form because of enhanced kinetics and stability. Herein, recent progress in developing transition-metal-based HER/OER electrocatalytic materials is reviewed with selected examples of chalcogenides, phosphides, carbides, nitrides, alloys, phosphates, oxides, hydroxides, and oxyhydroxides. Focusing on self-supported electrodes, the latest advances in their structural design, controllable synthesis, mechanistic understanding, and strategies for performance enhancement are presented. Remaining challenges and future perspectives for the further development of self-supported electrocatalysts are also discussed.
1,015 citations
TL;DR: The synthesis of dual-cation (Fe, Co)-incorporated NiSe2 nanosheets ( Fe, Co-NiSe2) and systematical investigation of their electrocatalytic performance for water splitting as a function of the composition are reported.
Abstract: Exploring highly efficient and low-cost electrocatalysts for electrochemical water splitting is of importance for the conversion of intermediate energy. Herein, the synthesis of dual-cation (Fe, Co)-incorporated NiSe2 nanosheets (Fe, Co-NiSe2 ) and systematical investigation of their electrocatalytic performance for water splitting as a function of the composition are reported. The dual-cation incorporation can distort the lattice and induce stronger electronic interaction, leading to increased active site exposure and optimized adsorption energy of reaction intermediates compared to single-cation-doped or pure NiSe2 . As a result, the obtained Fe0.09 Co0.13 -NiSe2 porous nanosheet electrode shows an optimized catalytic activity with a low overpotential of 251 mV for oxygen evolution reaction and 92 mV for hydrogen evolution reaction (both at 10 mA cm-2 in 1 m KOH). When used as bifunctional electrodes for overall water splitting, the current density of 10 mA cm-2 is achieved at a low cell voltage of 1.52 V. This work highlights the importance of dual-cation doping in enhancing the electrocatalyst performance of transition metal dichalcogenides.
342 citations
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TL;DR: It is anticipated that this review can stimulate a new research doorway to facilitate the next generation of g-C3N4-based photocatalysts with ameliorated performances by harnessing the outstanding structural, electronic, and optical properties for the development of a sustainable future without environmental detriment.
Abstract: As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and “earth-abundant” nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C3N4 and g-C3N4-based nanocomposites, including (1) nanoarchitecture design of bare g-C3N4, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C3N4 at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C3N4 with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The constructi...
5,054 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: Identifying and building a sustainable energy system are perhaps two of the most critical issues that today's society must address.
Abstract: Identifying and building a sustainable energy system are perhaps two of the most critical issues that today's society must address. Replacing our current energy carrier mix with a sustainable fuel is one of the key pieces in that system. Hydrogen as an energy carrier, primarily derived from water, can address issues of sustainability, environmental emissions, and energy security. Issues relating to hydrogen production pathways are addressed here. Future energy systems require money and energy to build. Given that the United States has a finite supply of both, hard decisions must be made about the path forward, and this path must be followed with a sustained and focused effort.
4,824 citations
TL;DR: In this article, a selective solvothermal synthesis of MoS2 nanoparticles on reduced graphene oxide (RGO) sheets suspended in solution was developed, which exhibited superior electrocatalytic activity in the hydrogen evolution reaction (HER).
Abstract: Advanced materials for electrocatalytic and photoelectrochemical water splitting are central to the area of renewable energy. In this work, we developed a selective solvothermal synthesis of MoS2 nanoparticles on reduced graphene oxide (RGO) sheets suspended in solution. The resulting MoS2/RGO hybrid material possessed nanoscopic few-layer MoS2 structures with an abundance of exposed edges stacked onto graphene, in strong contrast to large aggregated MoS2 particles grown freely in solution without GO. The MoS2/RGO hybrid exhibited superior electrocatalytic activity in the hydrogen evolution reaction (HER) relative to other MoS2 catalysts. A Tafel slope of ∼41 mV/decade was measured for MoS2 catalysts in the HER for the first time; this exceeds by far the activity of previous MoS2 catalysts and results from the abundance of catalytic edge sites on the MoS2 nanoparticles and the excellent electrical coupling to the underlying graphene network. The ∼41 mV/decade Tafel slope suggested the Volmer–Heyrovsky mec...
4,370 citations
TL;DR: Research in materials science is contributing to progress towards a sustainable future based on clean energy generation, transmission and distribution, the storage of electrical and chemical energy, energy efficiency, and better energy management systems.
Abstract: Civilization continues to be transformed by our ability to harness energy beyond human and animal power. A series of industrial and agricultural revolutions have allowed an increasing fraction of the world population to heat and light their homes, fertilize and irrigate their crops, connect to one another and travel around the world. All of this progress is fuelled by our ability to find, extract and use energy with ever increasing dexterity. Research in materials science is contributing to progress towards a sustainable future based on clean energy generation, transmission and distribution, the storage of electrical and chemical energy, energy efficiency, and better energy management systems.
2,894 citations