Designing ingenious and stable carbon nanostructures is critical but still challenging for use in energy storage devices with superior electrochemistry kinetics, durable capacitive activity, and high rate survivability. To pursue the objective, a simple self-assembly strategy is developed to access carbon superstructures built of nanoparticle embedded plates. The carbon precursors, 2,4,6-trichloro-1,3,5-triazine and 2,6-diaminoanthraquinone can form porous organic polymer with "protic salt"-type rigid skeleton linked by -NH2+ Cl- - "rivets", which provides the cornerstone for hydrogen-bonding-guided self-assembly of the organic backbone to superstructures by π-π plane stacking. The ameliorative charge density distribution and decreased adsorption energy in as-fabricated carbon superstructures allow the high accessibility of the build-in protophilic sites and efficient ion diffusion with a low energy barrier. Such superstructures thus deliver ultra-stable charge storage and fast proton-coupled kinetics at the structural-chemical defects, contributing to unprecedented lifespan (1 000 000 cycles), high-rate capability (100 A g-1 ) for carbon-based supercapacitors, and an ultrahigh energy density (128 Wh kg-1 ) for Zn-ion hybrid supercapacitors. The self-assembled carbon superstructures significantly improve the all-round electrochemical performances, and hold great promise for efficient energy storage.

Self-Assembled Carbon Superstructures Achieving Ultra-Stable and Fast Proton-Coupled Charge Storage Kinetics.

Green activation of sustainable resources to synthesize nitrogen-doped oxygen-riched porous carbon nanosheets towards high-performance supercapacitor

Metal phosphides (MPs) with unique and desirable physicochemical properties provide promising potential in practical applications, such as the catalysis, gas/humidity sensor, environmental remediation, and energy storage fields, especially for transition metal phosphides (TMPs) and MPs consisting of group IIIA and IVA metal elements. Most studies, however, on the synthesis of MP nanomaterials still face intractable challenges, encompassing the need for a more thorough understanding of the growth mechanism, strategies for large-scale synthesis of targeted high-quality MPs, and practical achievement of functional applications. This review aims at providing a comprehensive update on the controllable synthetic strategies for MPs from various metal sources. Additionally, different passivation strategies for engineering the structural and electronic properties of MP nanostructures are scrutinized. Then, we showcase the implementable applications of MP-based materials in emerging sustainable catalytic fields including electrocatalysis, photocatalysis, mild thermocatalysis, and related hybrid systems. Finally, we offer a rational perspective on future opportunities and remaining challenges for the development of MPs in the materials science and sustainable catalysis fields.

Nanostructured metal phosphides: from controllable synthesis to sustainable catalysis.

A robust strategy of solvent choice to synthesize optimal nanostructured carbon for efficient energy storage

Exploring porous electrode materials with designed micro/nano-structures is an effective way to realize high-performance supercapacitors (SCs). A metal-organic framework (MOF) is a porous crystalline material with a periodic structure formed by coordination of metal ions/clusters and organic ligands. Due to the excellent properties (e.g., large specific surface area, high porosity and tailorable structure), MOFs have been widely used in diverse applications. This Frontier article highlights the recent progress in the synthesis of MOF-based micro/nano-structured electrode materials including pristine MOFs, MOF composites and MOF derivatives, and their application in SCs. Furthermore, the challenges of MOF-based electrode materials and possible solutions are also discussed.

Recent advances in metal–organic framework-based electrode materials for supercapacitors

Fabrication of Ordered Macro-Microporous Single-Crystalline MOF and Its Derivative Carbon Material for Supercapacitor

Exploitation of high-efficiency and low-cost catalysts for dehydrogenation of the ideal hydrogen storage material (ammonia borane) can effectively promote the development of hydrogen economy. Here, we report an efficient and economical non-noble-metal magnetic catalyst (Ni0.23Co0.19P0.58@NHPC900) with nanoparticles uniformly distributed on MOF-derived (metal-organic framework) nitrogen-doped hierarchical porous carbon (NHPC900) by a one-step in situ synthesis method. The catalyst has achieved a superior initial total turnover frequency (TOF) of 125.2 molH2·molcat-1·min-1. Based on isotopic analyses and ion effects, we further obtain an unprecedentedly higher TOF of 282.4 molH2·molcat-1·min-1, the highest among non-noble-metal heterogeneous systems. Through experiments and theoretical studies, we confirm that the highly doped phosphorus component leads to a C-P-Ni-Co quaternary synergy in the catalyst. Then, the induced strong electron transfer and increased partial charge can reduce the reaction energy barrier, strengthen the adsorption of ammonia borane, and ultimately result in superior catalytic performance. The proposed mechanisms and strategies are helpful to develop non-noble-metal catalysts for practical applications of hydrogen energy systems in the future.

Highly Phosphatized Magnetic Catalyst with Electron Transfer Induced by Quaternary Synergy for Efficient Dehydrogenation of Ammonia Borane

Hierarchically porous CoP@CNR nanorod derived from metal-organic frameworks as noble-metal-free catalyst for dehydrogenization of ammonia-borane

Fabricating large-scale nanoarrays is a significant and challenging work in the field of nanometer devices. Anodic aluminum oxide (AAO) membrane is considered as a promising mask due to its inherent advantages such as low-cost and tunable pore diameter. However, there are few reports on the use of non-through-hole large-area AAO membrane as a mask. Due to its higher mechanical strength, non-through-hole AAO membrane has the advantage of self-supporting for large-area fabrication. Herein, we present a robust approach to transferring nanopattern to substrates with high fidelity by using the non-through-hole AAO membrane as an etching mask. A novel two-step inductively coupled plasma (ICP) etching method is adopted. The morphological evolution of the AAO during ICP etching is systematically investigated. The aspect ratio of the AAO can be quantitatively controlled by adjusting etching time. The AAO nanopore arrays with an area of 7.1 cm2 are successfully transferred to gallium nitride wafer to enhance photoluminescence. The luminous intensity of the nano-array LED with a pore diameter of 400 nm and a depth of 150 nm is improved by 3.4 times compared with the LED without the nano-array. This method extends the opportunities for AAO mask to serve as generic templates for novel applications that are previously impractical due to the difficulty of large-scale nano-pattern transfer.

https://iopscience.iop.org/article/10.1088/1361-6528/ab5b36/pdf

Weizhe Wang

Papers

Fabrication of Ordered Macro-Microporous Single-Crystalline MOF and Its Derivative Carbon Material for Supercapacitor

Highly Phosphatized Magnetic Catalyst with Electron Transfer Induced by Quaternary Synergy for Efficient Dehydrogenation of Ammonia Borane

Hierarchically porous CoP@CNR nanorod derived from metal-organic frameworks as noble-metal-free catalyst for dehydrogenization of ammonia-borane

Large-scale pattern transfer based on non-through-hole AAO self-supporting membranes.

Morphology- and size-dependent FAPbBr3/WO3 Z-scheme photocatalysts for the controllable photo-oxidation of benzyl alcohol