Zeolitic imidazolate frameworks (ZIFs), an important subfamily of metal–organic frameworks (MOFs), have been a hot topic as the porous structure nature, high specific surface area and abundant metal/metal compound active sites enables numerous applications in photo/electrocatalysis, gas storage, separation, and sensors etc. Also, ZIFs can serve as ideal precursors to synthesize versatilely functional materials based on the conversion of metal nodes and organic linkers. The microscopic morphology, size, and pore structure of ZIFs have a great influence on the applications. Therefore, it is important to design and synthesize ZIFs with different morphologies. Compared with direct nucleation in liquid phase, hard template strategy toward ZIFs provides a favorable opportunity to expand the microscopic morphology of ZIFs and their derivatives, from sphere, one-dimensional (1D) tube, two-dimensional (2D) sheet and three-dimensional (3D) flower, etc. Several works have summarized the synthesis and applications of ZIFs and its derivatives. However, there is a scarcity of reviews about the preparation of the ZIFs by the template method in the last 5 years. Here, this review focuses on hard-template based strategies for designing ZIFs and their derived materials. We first introduce the basic principles of ZIFs synthesized by the template method. Then, we summarize the types of templates and their advantages for synthesis. The corresponding routes used to synthesize different structures of ZIFs are described in detail. The influence of ZIF composition and structure on their applications in typical fields is also discussed. Finally, we present some challenges for the synthesis of ZIFs by the template method. This review will guide future research on constructing ZIFs with appropriate templates to extend their properties and applications. 

Recent advances in tailoring zeolitic imidazolate frameworks (ZIFs) and their derived materials based on hard template strategy for multifunctional applications

Herein, we report a versatile solvent-mediated polymerization-induced self-assembly (PISA) strategy to directly synthesize highly N-doped hierarchically porous structured carbon spheres with a tunable meso-macroporous configuration. The introduction of intermolecular hydrogen bonds is verified to enhance the interfacial interactions between block copolymers, oil droplets, and polyphenols. Moreover, the dominant hydrogen-bond-driven interactions can be systematically manipulated by selecting different cosolvent systems to generate diverse porous structures from the transformation of micellar and precursor co-assembly. Impressively, hierarchically structured meso-macroporous N-doped carbon spheres present simultaneously tunable sphere sizes and mesopores and macropores, ranging from 1.2 μm, 9/50 and 227 nm to 1.0 μm, 40, and 183 nm and 480, 24, and 95 nm. As a demonstration, dendritic-like N-doped hierarchically meso-macroporous carbon spheres manifest excellent enzyme-like activity, which is attributed to the continuous mass transport from the multiordered porosity. The current study provides a new platform for the synthesis of novel well-defined porous materials.

Tunable Hierarchically Structured Meso-Macroporous Carbon Spheres from a Solvent-Mediated Polymerization-Induced Self-Assembly.

Electrochemical nitrite-to-ammonia reduction (NO2RR) represents an attractive method to simultaneously attain hazardous NO2− removal and renewable NH3 synthesis. In this study, we first design single-atom Zn anchored on MnO2 nanowires (Zn1/MnO2) as a highly active and durable NO2RR catalyst. Atomic-scale characterizations reveal that Zn single atoms are coordinated with three surface-O atoms of MnO2 to form Zn1-O3 units. A combination of in situ electrochemical measurements and theoretical computations unravel that Zn1-O3 units enhance the NO2− activation, stabilize the key intermediate of *NHO and lower the energy barrier of NO2−-to-NH3 hydrogenation process. Consequently, Zn1/MnO2 assembled in a special flow cell reactor achieves the highest NH3 yield rate of 1559.1 μmol h−1cm−2 and NH3-Faradaic efficiency of 95.3 % at −288.5 mA cm−2, superior to nearly all previously reported NO2RR electrocatalysts. 

Single-atom Zn on MnO2 for selective nitrite electrolysis to ammonia

Well-orchestrated carbon nanostructure with superb stable framework and high surface accessibility is crucial for zinc-ion hybrid capacitors (ZIHCs). Herein, a hydrogen-bonded micelle self-assembly strategy is proposed for morphology-controllable synthesis of conjugated microporous polymers (CMPs) derived carbon to boost zinc ion storage capability. In the strategy, F127 micellar assembly through intermolecular hydrogen bonds serves as structure-directed agent, directing CMPs' oligomers grow into nanospherical assembly. The nanospherical carbon frameworks derived from CMPs (CNS-2) have shown maximized surface accessibility due to their plentiful tunable porosity and hierarchical porous structure with abundant mesoporous interconnected channels, and superb stability originating from CMPs' robust framework, thus the CNS-2-based ZIHCs exhibit ultrahigh energy density of 163 Wh kg−1 and ultralong lifespan with 93 % capacity retention after 200, 000 cycles at 20 A g−1. Charged ion storage efficiency also lies in dual-ion alternate uptake of Zn2+ and CF3SO3− as well as chemical redox of Zn2+ with carbonyl/pyridine motifs forming O–Zn–N bonds. Maximized surface accessibility and dual-ion storage mechanism ensure excellent electrochemical performance. Thus, the hydrogen-bond-guide micelle self-assembly strategy has provided a facile way to design nanoarchitectures of CMPs derived carbon for advanced cathodes of ZIHCs. 

Hydrogen-bonded micelle assembly directed conjugated microporous polymers for nanospherical carbon frameworks towards dual-ion capacitors

Abstract Designing effective electrocatalysts tailored for targeted reactions requires fundamental insights into the structure dependence of the reaction microenvironment. Herein, inspired by finite element simulations, N,O co‐doped carbon nanosheets featuring a hierarchical micro/mesoporous structure to form an oxygen‐rich and local alkaline‐like microenvironment for the two‐electron oxygen reduction reaction (2e − ORR) in a neutral medium are designed. The in situ and ex situ test results confirmed that the micro/mesoporous carbon architecture can elevate the local pH and accelerate the generation of intermediates (*O 2 , *OOH), leading to high‐efficiency H 2 O 2 production. Utilizing this favorable microenvironment, N,O‐CNS 0.5 demonstrated exceptional H 2 O 2 electrosynthesis performance in neutral media, achieving a superior H 2 O 2 yield rate (6705 mmol g catalyst −1 h −1 in a flow cell). Additionally, comparative experiments and density‐functional theory calculations provided confirmation of the bi‐doping of N and O as the active origin responsible for the electrochemical 2e − ORR. This study synergistically manipulates the reaction microenvironment and active sites, providing an opportunity for efficient H 2 O 2 electro‐production in a neutral medium. 

Unveiling Favorable Microenvironment on Porous Doped Carbon Nanosheets for Superior H2O2 Electrosynthesis in Neutral Media

Single-atom Zn with nitrogen defects on biomimetic 3D carbon nanotubes for bifunctional oxygen electrocatalysis.

Controlled Fabrication of Polydopamine Nanocapsules via Polymerization-Induced Self-Assembly

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Tunable Hierarchically Structured Meso-Macroporous Carbon Spheres from a Solvent-Mediated Polymerization-Induced Self-Assembly.

Single-atom Zn with nitrogen defects on biomimetic 3D carbon nanotubes for bifunctional oxygen electrocatalysis.

Controlled Fabrication of Polydopamine Nanocapsules via Polymerization-Induced Self-Assembly