As emerging crystalline porous organic-inorganic hybrid materials, metal-organic frameworks (MOFs) have been widely used as sacrificial precursors for the synthesis of carbon materials, metal/metal compounds, and their composites with tunable and controllable nanostructures and chemical compositions for electrochemical energy applications. Herein, recent progress of MOF-derived nanomaterials for various electrochemical energy storage and conversion applications including Li-ion batteries, Li-S batteries, Na-ion batteries, supercapacitors, water splitting, and oxygen reduction reaction is reviewed. Structural and compositional design of MOF-derived nanomaterials is systematically summarized, which may hopefully offer inspirations and guidances for future development of MOF-derived nanomaterials for more efficient and more durable electrochemical energy applications.

Metal-organic framework-derived materials for electrochemical energy applications

Electrochemical water splitting has attracted significant attention as a key pathway for the development of renewable energy systems. Fabricating efficient electrocatalysts for these processes is intensely desired to reduce their overpotentials and facilitate practical applications. Recently, metal-organic framework (MOF) nanoarchitectures featuring ultrahigh surface areas, tunable nanostructures, and excellent porosities have emerged as promising materials for the development of highly active catalysts for electrochemical water splitting. Herein, the most pivotal advances in recent research on engineering MOF nanoarchitectures for efficient electrochemical water splitting are presented. First, the design of catalytic centers for MOF-based/derived electrocatalysts is summarized and compared from the aspects of chemical composition optimization and structural functionalization at the atomic and molecular levels. Subsequently, the fast-growing breakthroughs in catalytic activities, identification of highly active sites, and fundamental mechanisms are thoroughly discussed. Finally, a comprehensive commentary on the current primary challenges and future perspectives in water splitting and its commercialization for hydrogen production is provided. Hereby, new insights into the synthetic principles and electrocatalysis for designing MOF nanoarchitectures for the practical utilization of water splitting are offered, thus further promoting their future prosperity for a wide range of applications.

Designing MOF Nanoarchitectures for Electrochemical Water Splitting.

In electrocatalysis, doping regulation has been considered as an effective method to modulate the active sites of catalysts, providing a powerful means for creating a large variety of highly efficient catalysts for various reactions. Of particular interest, there has been growing research concerning the doping of two-dimensional transition-metal compounds (TMCs) to optimize their electrocatalytic performance. Despite the previous achievements, mechanistic insights of doping regulation in TMCs for electrocatalysis are still lacking. Herein, we provide a systematic overview of doping regulation in TMCs in terms of background, preparation, impacts on physicochemical properties, and typical applications including the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, CO2 reduction reaction, and N2 reduction reaction. Notably, we bridge the understanding between the doping regulation of catalysts and their catalytic activities via focusing on the physicochemical properties of catalysts from the aspects of vacancy concentrations, phase transformation, surface wettability, electrical conductivity, electronic band structure, local charge distribution, tunable adsorption strength, and multiple adsorption configurations. We also discuss the existing challenges and future perspectives in this promising field.

Doping regulation in transition metal compounds for electrocatalysis

Electrocatalytical nitrogen reduction reaction (NRR) under ambient conditions provides a promising substitute to the typical Haber−Bosch process that involves high energy and greenhouse gases emission. Herein, we develop non-noble metal based hollow hierarchical nanotubes (HHNTs) of CoVP@NiFeV-layered double hydroxides (LDHs) heterostructures as a high-performance electrocatalyst for NRR, in which the novel 3D hollow hierarchical structure provides highly rich surface active sites for the adsorption and reduction of nitrogen to NH3. Electrochemical measurements for NRR reveal high activity (NH3 rate: 1.6 × 10−6 mol h−1 cm−2), high Faradaic efficiency (13.8%) and excellent selectivity at −0.3 V versus reversible hydrogen electrode (RHE), outperforming other noble metals catalysts for N2 fixation and most of state-of-the-art metal-free NRR electrocatalysts. Furthermore, CoVP@NiFeV-LDHs HHNTs could maintain high selectivity and durability over repeated reaction cycles. Therefore, this work highlights the first example of CoVP@NiFeV-LDHs hierarchical micro/nanostructures, which serve as electrocatalysts towards high-efficiency, pH-universal NRR to ammonia synthesis.

Hierarchical hollow nanotubes of NiFeV-layered double hydroxides@CoVP heterostructures towards efficient, pH-universal electrocatalytical nitrogen reduction reaction to ammonia

Electrochemical splitting of water is an appealing solution for energy storage and conversion to overcome the reliance on depleting fossil fuel reserves and prevent severe deterioration of the global climate. Though there are several fuel cells, hydrogen (H2) and oxygen (O2) fuel cells have zero carbon emissions, and water is the only by-product. Countless researchers worldwide are working on the fundamentals, i.e. the parameters affecting the electrocatalysis of water splitting and electrocatalysts that could improve the performance of the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) and overall simplify the water electrolysis process. Noble metals like platinum for HER and ruthenium and iridium for OER were used earlier; however, being expensive, there are more feasible options than employing these metals for all commercialization. The review discusses the recent developments in metal and metalloid HER and OER electrocatalysts from the s, p and d block elements. The evaluation perspectives for electrocatalysts of electrochemical water splitting are also highlighted.

/pdf/a-comprehensive-review-on-the-electrochemical-parameters-and-qh8rc6yd.pdf

A comprehensive review on the electrochemical parameters and recent material development of electrochemical water splitting electrocatalysts

Searching for highly active and stable bifunctional electrocatalysts for overall water splitting, e.g., for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER), is dominating in terms of bringing future renewable energy storage and conversion processes to reality. In this work, a kind of two-dimensional ultrathin manganese (Mn) doped polyhedral cobalt phosphide (Mn-CoP) has been synthesized via the etching-carbonization-phosphidation of Co-centered metal-organic frameworks. The as-prepared porous Mn-CoP nanosheets had a larger specific surface area and higher porosity, furnishing them with more plentiful catalytically active sites than their counterpart hollow CoP and Mn-CoP nanoparticles, and thus showed much better electrocatalytic activity for both HER and OER in acidic and alkaline media. In addition, the Mn-CoP nanosheets also demonstrated excellent durability after long-term operation. These high performances are attributed to the synergistic effects of the CoP nanosheets with intrinsic activity, the graphitic carbon and the controllable electronic structure doped by Mn and N elements. This synthetic methodology of using a classical MOF as a precursor to build a new 2D sheet-like composite may create opportunities to search for highly efficient and robust non-precious metal catalysts for energy-related reactions.

MOF-derived Mn doped porous CoP nanosheets as efficient and stable bifunctional electrocatalysts for water splitting

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MOF-derived Mn doped porous CoP nanosheets as efficient and stable bifunctional electrocatalysts for water splitting