Flexible solid-state supercapacitors (FSSCs) are frontrunners in energy storage device technology and have attracted extensive attention owing to recent significant breakthroughs in modern wearable electronics In this study, we review the state-of-the-art advancements in FSSCs to provide new insights on mechanisms, emerging electrode materials, flexible gel electrolytes and novel cell designs The review begins with a brief introduction on the fundamental understanding of charge storage mechanisms based on the structural properties of electrode materials The next sections briefly summarise the latest progress in flexible electrodes (ie, freestanding and substrate-supported, including textile, paper, metal foil/wire and polymer-based substrates) and flexible gel electrolytes (ie, aqueous, organic, ionic liquids and redox-active gels) Subsequently, a comprehensive summary of FSSC cell designs introduces some emerging electrode materials, including MXenes, metal nitrides, metal–organic frameworks (MOFs), polyoxometalates (POMs) and black phosphorus Some potential practical applications, such as the development of piezoelectric, photo-, shape-memory, self-healing, electrochromic and integrated sensor-supercapacitors are also discussed The final section highlights current challenges and future perspectives on research in this thriving field

Towards flexible solid-state supercapacitors for smart and wearable electronics

Supercapacitors have gained a lot of attention due to their unique features like high power, long cycle life and environment-friendly nature. They act as a link for energy-power difference between a traditional capacitor (having high power) and fuel cells/batteries (having high energy storage). In this perspective, a worldwide research has been reported to address this and rapid progress has been achieved in the advancement of fundamental as well as the applied aspects of supercapacitors. Here, a concise description of technologies and working principles of different materials utilized for supercapacitors has been provided. The main focus has been on materials like carbon-based nanomaterials, metal oxides, conducting polymers and their nanocomposites along with some novel materials like metal-organic frameworks, MXenes, metal nitrides, covalent organic frameworks and black phosphorus. The performance of nanocomposites has been analysed by parameters like energy, capacitance, power, cyclic performance and rate capability. Some of the latest supercapacitors such as electrochromic supercapacitor, battery-supercapacitor hybrid device, electrochemical flow capacitor, alternating current line filtering capacitor, micro-supercapacitor, photo-supercapacitor, thermally chargeable supercapacitor, self-healing supercapacitor, piezoelectric and shape memory supercapacitor have also been discussed. This review covers the up-to-date progress achieved in novel materials for supercapacitor electrodes. The latest fabricated symmetric/asymmetric supercapacitors have also been reported.

Review of supercapacitors: Materials and devices

Oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are three key reactions for the development of green and sustainable energy systems. Efficient electrocatalysts for these reactions are highly desired to lower their overpotentials and promote practical applications of related energy devices. Metal–organic frameworks (MOFs) have recently emerged as precursors to fabricate carbon-based electrocatalysts with high electrical conductivity and uniformly distributed active sites. In this review, the current progress of MOF-derived carbon-based materials for ORR/OER/HER electrocatalysis is presented. Materials design strategies of MOF-derived carbon-based materials are firstly summarized to show the rich possibilities of the morphology and composition of MOF-derived carbon-based materials. A wide range of applications based on these materials for ORR, OER, HER and multifunctional electrocatalysis are discussed, with an emphasis on the required features of MOF-derived carbon-based materials for the electrocatalysis of corresponding reactions. Finally, perspectives on the development of MOF-derived carbon-based materials for ORR, OER and HER electrocatalysis are provided.

MOF-derived electrocatalysts for oxygen reduction, oxygen evolution and hydrogen evolution reactions

Replacing the rare and precious platinum (Pt) electrocatalysts with earth-abundant materials for promoting the oxygen reduction reaction (ORR) at the cathode of fuel cells is of great interest in developing high-performance sustainable energy devices. However, the challenging issues associated with non-Pt materials are still their low intrinsic catalytic activity, limited active sites, and the poor mass transport properties. Recent advances in material sciences and nanotechnology enable rational design of new earth-abundant materials with optimized composition and fine nanostructure, providing new opportunities for enhancing ORR performance at the molecular level. This Review highlights recent breakthroughs in engineering nanocatalysts based on the earth-abundant materials for boosting ORR.

Earth-Abundant Nanomaterials for Oxygen Reduction.

This review captures the synthesis, assembly, properties, and applications of copper chalcogenide NCs, which have achieved significant research interest in the last decade due to their compositional and structural versatility. The outstanding functional properties of these materials stems from the relationship between their band structure and defect concentration, including charge carrier concentration and electronic conductivity character, which consequently affects their optoelectronic, optical, and plasmonic properties. This, combined with several metastable crystal phases and stoichiometries and the low energy of formation of defects, makes the reproducible synthesis of these materials, with tunable parameters, remarkable. Further to this, the review captures the progress of the hierarchical assembly of these NCs, which bridges the link between their discrete and collective properties. Their ubiquitous application set has cross-cut energy conversion (photovoltaics, photocatalysis, thermoelectrics), en...

Compound Copper Chalcogenide Nanocrystals

Due to their unique electronic and optoelectronic properties, tin selenide nanostructures show great promise for applications in energy storage and photovoltaic devices. Despite the great progress that has been achieved, the phase-controlled synthesis of two-dimensional (2D) tin selenide nanostructures remains a challenge, and their use in supercapacitors has not been explored. In this paper, 2D tin selenide nanostructures, including pure SnSe2 nanodisks (NDs), mixed-phase SnSe–SnSe2 NDs, and pure SnSe nanosheets (NSs), have been synthesized by reacting SnCl2 and trioctylphosphine (TOP)-Se with borane-tert-butylamine complex (BTBC) and 1,3-dimethyl-3,4,5,6-tetrahydro-2(1H)-pyrimidinone. Utilizing the interplay of TOP and BTBC and changing only the amount of BTBC, the phase-controlled synthesis of 2D tin selenide nanostructures is realized for the first time. Phase-dependent pseudocapacitive behavior is observed for the resulting 2D nanostructures. The specific capacitances of pure SnSe2 NDs (168 F g–1) an...

Two-dimensional tin selenide nanostructures for flexible all-solid-state supercapacitors.

A novel MOF-templated nitrogen and sulphur co-doped porous material has been synthesized as an efficient electrocatalyst for oxygen reduction reactions (ORRs) for the first time. The representative NS(3 : 1)–C-MOF-5 catalyst shows the highest onset potential, and is even comparable to commercial Pt–C catalyst, due to the synergistic effect of N and S co-doping.

Metal–organic framework templated nitrogen and sulfur co-doped porous carbons as highly efficient metal-free electrocatalysts for oxygen reduction reactions

A novel in situ-generated nanogold plasmon-enhanced photoelectrochemical aptasensor for Hg2+ ions was fabricated using a perylene-3,4,9,10-tetracarboxylic acid/graphene (PTCA-GR) heterojunction. The fabricated photoelectrochemical aptasensor was based on thymine–Hg2+–thymine coordination chemistry and the plasmonic near-field absorption enhancement effect of the subsequent specific catalytic formation of nanogold. The energetic electrons from the surface plasmons of the nanogold were injected into the LUMO orbit of the organic PTCA semiconductor and then rapidly transferred to the electrode through GR due to the possible Hg2+-DNA molecular wires following irradiation with the visible light (λ > 450 nm) and at a bias voltage of 0.2 V. The fabricated aptasensor was linear in its response to the concentration of Hg2+ ions in the range of 5–500 pmol L–1, with a detection limit of 2 pmol L–1. The presence of up to 200-fold greater concentrations of other common metal ions did not interfere with the detection o...

In situ-generated nano-gold plasmon-enhanced photoelectrochemical aptasensing based on carboxylated perylene-functionalized graphene.

The rich phase structure of Cu2Se may provide good opportunities for modulating and optimizing their catalytic properties. However, chemical synthesis of Cu2Se nanostructures with different crystal...

Controllable Synthesis of Tetragonal and Cubic Phase Cu2Se Nanowires Assembled by Small Nanocubes and Their Electrocatalytic Performance for Oxygen Reduction Reaction

A label-free electrochemical biosensing platform has been developed for the first time using carbon nanotubes for facile detection of malondialdehyde, showing high sensitivity and acceptable selectivity with a low detection limit of 0.047 μmol L−1 and a linear response ranging from 0.1 to 90 μmol L−1.

Ya-Qian Lan

Papers

Two-dimensional tin selenide nanostructures for flexible all-solid-state supercapacitors.

Metal–organic framework templated nitrogen and sulfur co-doped porous carbons as highly efficient metal-free electrocatalysts for oxygen reduction reactions

In situ-generated nano-gold plasmon-enhanced photoelectrochemical aptasensing based on carboxylated perylene-functionalized graphene.

Controllable Synthesis of Tetragonal and Cubic Phase Cu2Se Nanowires Assembled by Small Nanocubes and Their Electrocatalytic Performance for Oxygen Reduction Reaction

Label-free and facile electrochemical biosensing using carbon nanotubes for malondialdehyde detection