Electrochemical supercapacitors process ultra–high power density and long lifetime, but the relatively low energy density hinder the wide application. Therefore, supercapacitors with high energy density and high power density (“dual high”) have attracted great attentions. New active materials with high pseudocapacitance beyond electronic double layer capacitance and novel devices with high working voltage, are two approaches toward “dual high” supercapacitors. In this review, we briefly introduce the history, classification, basic mechanism, and device architecture of supercapacitors. Then, the key issues and design strategies for “dual high” supercapacitors will be proposed. The recent methodical advances will also be highlighted on the material with outstanding specific capacitance and the corresponding electrolyte systems with expanded operating voltage. Besides, the recent progresses of current collectors and separators for supercapacitors are also included. Finally, we will provide our insights regarding the major challenges and prospective solutions in this highly exciting field. We believe such a review will significantly expand the horizons in ever-deepening understanding toward “dual high” supercapacitors 

Materials design and preparation for high energy density and high power density electrochemical supercapacitors

Metal-organic framework (MOF)-based materials, including pristine MOFs, MOF composites, and MOF derivatives, have become a research focus in energy storage and conversion applications due to their customizability, large specific surface area, and tunable pore size. However, MOF-based materials are currently in their infancy, and more efforts need to be dedicated to enable them to perform competitively in large-scale practical applications. This updated review provides an overview of the advances in MOF-based materials in energy storage and conversion applications, including gas storage, batteries, supercapacitors, and photo/electrochemical energy conversion, highlighting the advantages of different materials in various scenarios. Finally, we summarize the current challenges and status of MOF-based materials for energy storage and conversion and provide an outlook for future research directions. 

Metal-organic framework-based materials as platforms for energy applications

Electrocatalytic CO2 reduction reaction (CO2RR) in membrane electrode assembly (MEA) systems is a promising technology. Gaseous CO2 can be directly transported to the cathode catalyst layer, leading to enhanced reaction rate. Meanwhile, there is no liquid electrolyte between the cathode and the anode, which can help to improve the energy efficiency of the whole system. The remarkable progress achieved recently points out the way to realize industrially relevant performance. In this review, we focus on the principles in MEA for CO2RR, focusing on gas diffusion electrodes and ion exchange membranes. Furthermore, anode processes beyond the oxidation of water are considered. Besides, the voltage distribution is scrutinized to identify the specific losses related to the individual components. We also summarize the progress on the generation of different reduced products together with the corresponding catalysts. Finally, the challenges and opportunities are highlighted for future research.

Membrane Electrode Assembly for Electrocatalytic CO2 Reduction: Principle and Application.

Cu-based electrocatalysts have great potential for facilitating CO2 reduction to produce energy-intensive fuels and chemicals. However, it remains challenging to obtain high product selectivity due to the inevitable strong competition among various pathways. Here, we propose a strategy to regulate the adsorption of oxygen-associated active species on Cu by introducing an oxophilic metal, which can effectively improve the selectivity of C2+ alcohols. Theoretical calculations manifested that doping of Lewis acid metal Al into Cu can affect the C-O bond and Cu-C bond breaking toward the selectively determining intermediate (shared by ethanol and ethylene), thus prioritizing the ethanol pathway. Experimentally, the Al-doped Cu catalyst exhibited an outstanding C2+ Faradaic efficiency (FE) of 84.5% with remarkable stability. In particular, the C2+ alcohol FE could reach 55.2% with a partial current density of 354.2 mA cm-2 and a formation rate of 1066.8 μmol cm-2 h-1. A detailed experimental study revealed that Al doping improved the adsorption strength of active oxygen species on the Cu surface and stabilized the key intermediate *OC2H5, leading to high selectivity toward ethanol. Further investigation showed that this strategy could also be extended to other Lewis acid metals. 

Oxophilicity-Controlled CO2 Electroreduction to C2+ Alcohols over Lewis Acid Metal-Doped Cuδ+ Catalysts.

Large-scale deployment of proton exchange membrane (PEM) water electrolyzers has to overcome a cost barrier resulting from the exclusive adoption of platinum group metal (PGM) catalysts. Ideally, carbon-supported platinum used at cathode should be replaced with PGM-free catalysts, but they often undergo insufficient activity and stability subjecting to corrosive acidic conditions. Inspired by marcasite existed under acidic environments in nature, we report a sulfur doping–driven structural transformation from pyrite-type cobalt diselenide to pure marcasite counterpart. The resultant catalyst drives hydrogen evolution reaction with low overpotential of 67 millivolts at 10 milliamperes per square centimeter and exhibits no degradation after 1000 hours of testing in acid. Moreover, a PEM electrolyzer with this catalyst as cathode runs stably over 410 hours at 1 ampere per square centimeter and 60°C. The marked properties arise from sulfur doping that not only triggers formation of acid-resistant marcasite structure but also tailors electronic states (e.g., work function) for improved hydrogen diffusion and electrocatalysis.

https://www.science.org/doi/pdf/10.1126/sciadv.adh2885?download=true

Efficient acidic hydrogen evolution in proton exchange membrane electrolyzers over a sulfur-doped marcasite-type electrocatalyst

Delocalization state-induced selective bond breaking for efficient methanol electrosynthesis from CO2

Cold-Sintered Bi2Te3-Based Materials for Engineering Nanograined Thermoelectrics

Amorphous Lithium-Phosphate-Encapsulated Fe2O3 as a High-Rate and Long-Life Anode for Lithium-Ion Batteries

LiTMPO4 materials, such as LiNiPO4, can maintain structural stability and Li+ transport activity up to 4.8 V, showing great potential to stabilize layered nickel-rich cathodes at high voltage. But achieving a uniform LiTMPO4 coating layer remains a great challenge. Herein, an ultrathin and uniform LiTMPO4 layer (mainly LiNiPO4) is successfully coated on the surface of LiNi0.8Co0.15Mn0.05O2 (NMC@LTMP) via utilizing the surface chelation of phytic acid with NMC precursors and a subsequent high-temperature in situ reaction. The reconstructed surface and interface could act as stable paths for Li+ transport and efficient barriers against electrolyte corrosion. Thus, harmful side reactions like solid electrolyte interphase overgrowth, irreversible phase transformation, and metal dissolution are inhibited simultaneously. Impressively, the optimized NMC@LTMP2 cathode exhibits remarkably improved capacity, as high as 215 mA h g-1 at 2.8-4.5 V, with capacity retention of 87.21% after 200 cycles and outstanding rate capability of 140 mA h g-1 at 10C, significantly better than a pristine cathode. Furthermore, a pouch cell assembled with an NMC@LTMP2 cathode and graphite anode also exhibits robust capacity retention of 82.42% after 100 cycles. These results provide useful insights towards enabling the application of NMC cathodes via developing facile modification methods.

A uniform and high-voltage stable LiTMPO4 coating layer enabled high performance LiNi0.8Co0.15Mn0.05O2 towards boosting lithium storage.

Effective removal of the heavy metal ions down to the mark of tolerance concentration (parts per billion level) in drinking water remains a great challenge. Metal oxide-related materials has emerged...

A New Compound Mn5P4O20H8 Achieving Efficient Heavy Metals Removal to ppb Level through A Dual Chemisorption-ion exchange Pathway

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