Developing efficient and robust heterogeneous metallophthalocyanine electrocatalysts for CO2 reduction remains a challenge. Here, a general synthetic method of zinc-metallophthalocyanine (MPc) molecular layer/polyoxometalate (POM) sandwich lamellar material is developed, and thus improved performance of electrocatalytic and photocoupled electrocatalytic CO2 reduction is achieved. The incorporation of POM could prevent the packing of MPc molecular layers from aggregation, which would be favorable to the exposure of active sites. The molecular layer sandwich catalyst presents superior CO2 reduction activity, delivering the highest CO Faradaic efficiency (FECO) of 96.1% at -0.7 V vs RHE in dark field. Under light irradiation, over 93% FECO is achieved in a broad potential range from -0.6 to -0.9 V vs RHE with a maximum of 96.2%, and the carbon monoxide turnover frequency could exceed 2060 h-1. Photoelectrochemical tests and luminescence characterizations reveal the molecular layer is beneficial for carrier separation during light irradiation; density functional theory calculations and electron paramagnetic resonance indicated a 2-fold enhancement of the external light field on the catalytic performance.

Polyoxometalate Interlayered Zinc-Metallophthalocyanine Molecular Layer Sandwich as Photocoupled Electrocatalytic CO2 Reduction Catalyst.

Polymer dielectrics with high breakdown strength (Eb) and high efficiency are urgently demanded in advanced electrical and electronic systems, yet their energy density (Ue) is limited due to low dielectric constant (εr) and high loss at elevated temperatures. Conventional inorganic fillers with diameters from nano to micrometers can only increase εr at the cost of compromised Eb and Ue due to their poor compatibility with polymer matrix. Herein, hydroxyapatite (HAP) sub‐nanowires with a diameter of ≈0.9 nm are incorporated in polyetherimide (PEI) matrix to form HAP/PEI sub‐nanocomposites. εr and Eb of the composites are concomitantly enhanced with only 0.5 wt.% of HAP sub‐nanowires, leading to high Ue of 5.14 (@150 °C) and 3.1 J cm−3 (@200 °C) with efficiency of 90% and high‐temperature stability up to 3 × 105 charge‐discharge cycles at 200 °C. Microstructural analysis and molecular dynamics simulations indicate that the sub‐nanowires with comparable diameter as polymer chains induce enormous interfacial area, substantially increase mobility of polymer chains and form dense traps for charge carriers. This work extends the current research scope of polymer‐inorganics composite dielectrics to the sub‐nano‐level incorporation and provides a novel strategy for fabricating high performance polymer dielectrics at elevated temperatures.

Sub‐Nanowires Boost Superior Capacitive Energy Storage Performance of Polymer Composites at High Temperatures

Sub-nanometric materials (SNMs) are an attractive scope in recent years due to their atomic-level size and unique properties. Among various performances of SNMs, photothermal energy conversion is one of the most important ones because it can efficiently utilize the light energy. Herein, the SNMs with photothermal energy conversion behaviors and their applications are reviewed. First, a hydrothermal/solvothermal method for the synthesis of SNMs is systematically discussed, including the LaMer pathway and the cluster-nuclei coassembly pathway. Based on this synthetic strategy, many kinds of SNMs with different morphologies are successfully prepared, such as nanorings, nanowires, nanosheets, and nanobelts. These SNMs exhibit excellent photothermal performance under the laser or solar irradiation according to their different light absorption ranges. These enhanced absorption performances of SNMs are induced by the mechanism of plasmonic localized heating or nonradiative relaxation. Finally, the applications of the photothermal SNMs are illustrated. The SNMs with photothermal behaviors can be widely applied in the fields of solar vapor generation, biomedicine, and light-responsive composites construction. It is hoped that this review can provide new viewpoints and profound understanding to the SNMs in photothermal energy conversion.

Recent Progress of Sub-Nanometric Materials in Photothermal Energy Conversion

Polyoxometalate (POM) clusters with atomic precision structures are promising candidates construct functional nanomaterials via self-assembly. Non-covalent interactions at molecular levels can govern the self-assembly of POM clusters, for which the precise control of POM-based assemblies can be realized at single-cluster levels. This mini-review focuses on the synthesis and properties of POM-based nanostructures, including amphiphilic POM assemblies and co-assemblies of POM clusters and other subnanometer building blocks. Several synthetic strategies have been developed for rational control of POM-based assemblies in terms of morphologies, compositions and properties. 1D subnanometer POM assemblies demonstrate remarkable enhanced mechanical properties due to the topological interactions between nanowires and surroundings. The in-depth understanding of POM-based assemblies may help in the design of functional nanomaterials in fundamental perspectives and applications. 

Precise Assembly of Polyoxometalates at Single‐cluster Levels

Polyoxometalate (POM) clusters with atomic precision structures are promising candidates construct functional nanomaterials via self-assembly. Non-covalent interactions at molecular levels can govern the self-assembly of POM clusters, for which the precise control of POM-based assemblies can be realized at single-cluster levels. This mini-review focuses on the synthesis and properties of POM-based nanostructures, including amphiphilic POM assemblies and co-assemblies of POM clusters and other subnanometer building blocks. Several synthetic strategies have been developed for rational control of POM-based assemblies in terms of morphologies, compositions and properties. 1D subnanometer POM assemblies demonstrate remarkable enhanced mechanical properties due to the topological interactions between nanowires and surroundings. The in-depth understanding of POM-based assemblies may help in the design of functional nanomaterials in fundamental perspectives and applications.

Precise Assembly of Polyoxometalates at Single-cluster Levels.

Here it is shown that polyoxometalate (POM) clusters (H3 PW12 O40 ·xH2 O, PW12 ) can be introduced to interact with Au nanoclusters to form the "A-B-A-B" type building block ("A" represents Au nanoclusters and "B" stands for PW12 clusters), which continue to grow into copolymer-analogue Au-PW12 sub-1 nm nanowires. Due to the synergetic effect of Au nanoclusters and POMs, the obtained Au-PW12 sub-1 nm nanowires efficiently perform catalytic activity in the photo-electrochemical converting CO2 into CO. Under light, the catalyst maintains remarkable faradic efficiency (FE) of ≈99% from -0.7 to -0.9V (RHE), which is better than that in dark (FE of 66.4-90.64% from -0.7 to -0.9 V (RHE)). Density functional theory calculations and cryo-electron microscope images support the "A-B-A-B" type of structure and mechanistic studies also reveal the higher reactivity toward COOH* formation and CO adsorption on the catalyst, which lead to the superior catalytic activity in CO2 reduction reaction.

Au‐Polyoxometalates A‐B‐A‐B Type Copolymer‐Analogue Sub‐1 nm Nanowires

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Au‐Polyoxometalates A‐B‐A‐B Type Copolymer‐Analogue Sub‐1 nm Nanowires