The field of synthetic metals was, and remains, highly influential for the development of organic semiconductor materials. Yet, with the passing of time and the rapid development of conjugated materials in recent years, the link between synthetic metals and organic semiconductors is at risk of being forgotten. In this review, we reflect on one of the key concepts developed in synthetic metals - heteroatom interactions. The application of this strategy in recent organic semiconductor materials, small molecules and polymers, is highlighted, with analysis of X-ray crystal structures and comparisons with model systems used to determine the influence of these non-covalent short contacts. The case is made that the wide range of effective heteroatom interactions and the high performance that has been achieved in devices from organic solar cells to transistors is testament to the seeds sown by the synthetic metals research community. This article is protected by copyright. All rights reserved.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/adma.202302259

Lest we Forget - the Importance of Heteroatom Interactions in Heterocyclic Conjugated Systems, from Synthetic Metals to Organic Semiconductors.

Featured with the attractive properties such as large surface area, unique atomic layer thickness, excellent electronic conductivity, and superior catalytic activity, layered metal chalcogenides (LMCs) have received considerable research attention in electrocatalytic applications. In this review, the approaches developed to synthesize LMCs-based electrocatalysts are summarized. Recent progress in LMCs-based composites for electrochemical energy conversion applications including oxygen reduction reaction, carbon dioxide reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, overall water splitting, and nitrogen reduction reaction is reviewed, and the potential opportunities and practical obstacles for the development of LMCs-based composites as high-performing active substances for electrocatalytic applications are also discussed. This review may provide an inspiring guidance for developing high-performance LMCs for electrochemical energy conversion applications.

Synthesis and Electrocatalytic Applications of Layer-Structured Metal Chalcogenides Composites.

Transition metal phosphides (TMPs) with platinum like electronic structures are becoming a potential choice to constructing bifunctional catalysts operated under alkaline conditions. Nevertheless, the instability of TMP prevents a further enhancement on its electrocatalytic activity. In this study, the Co3O4 core was first formed through thermal annealing in air, and then the outer NiPx layer was formed through the P-method, cleverly integrating the properties of the inner and outer materials and supplementing respective shortcomings, ultimately improving their water decomposition performance. When Co3O4@NiPx is used as a bifunctional electrocatalyst in 1 M KOH, the HER performance is determined to be 99 mV (η10). The electrocatalytic performance for oxygen evolution reaction (OER) is 249 mV (η50). For overall water decomposition, the bifunctional electrocatalysts Co3O4@NiPx coupled dual electrode alkaline battery only requires 1.51 V to obtain η50 and maintains its excellent electrocatalytic ability for 50 h. Finally, a combination of electrostatic field theory analysis and DFT calculations was used, the results indicated that the stability of core–shell materials can be significantly enhanced through Co3O4 core and internal electron redistribution by P atoms, thereby improving catalytic performance. The greatly improved electrochemical performance of Co3O4@NiPx indicates the rationality of the design and synthesis of the core–shell structure. The combination of electrostatic field theory analysis and DFT calculation also further reveals the rationality of its internal electrocatalytic mechanism. 

Theoretical and experimental investigation on electrostatic field dynamics of Co3O4@NiPx electrocatalyst with core shell structure in overall water splitting reactions

Nanorobots are being received with a great attention for their move‐sense‐and‐act capabilities that often originate from catalytic decomposition of fuels. In the past decade, single‐atom engineering has demonstrated exceptional efficiency in catalysis, energy‐related technologies, and medicine. Here, a novel approach involving point defect engineering and the incorporation of platinum (Pt) single atoms and atomic level species onto the surface of titanium dioxide nanotubes (TiO2‐NT)‐based nanorobots is presented and its impact on the propulsion capabilities of the resulting nanorobots is investigated. The achievement of point defect engineering is realized through the annealing of TiO2‐NT in a hydrogen atmosphere yielding to the point‐defect decorated nanotube (TiO2‐HNT) nanorobots. Subsequently, the atomic level Pt species decorated TiO2 nanotube (TiO2‐SA‐NT) nanorobots are achieved through a wet‐chemical deposition process.  Whereas TiO2‐SA‐NT nanorobots showed the highest negative photogravitaxis when irradiated with ultraviolet (UV) light, TiO2‐HNT nanorobots reached the highest velocity calculated in 2D. Both TiO2‐HNT and TiO2‐SA‐NT nanorobots demonstrated a pronounced affinity for microplastics, exhibiting the capability to irreversibly capture them. This pioneering approach utilizing point‐defect and atomic level Pt species nanorobotics is anticipated to pave the way for highly efficient solutions in the remediation of nano‐ and microplastics and related environmental technologies.

Precision Engineering of Nanorobots: Toward Single Atom Decoration and Defect Control for Enhanced Microplastic Capture

Color Design for Daytime Radiative Cooling: Fundamentals and Approaches

Effect of Modified Thiophene Anchor on Molecule-Electrode Bonding

Creating through-space electron transport (ET) channels in the molecular backbone has been rarely explored in molecular electronics. Here, we demonstrated that through-space channels could be readily created by substituting the H atom of the central benzene in a starting molecule 1,4-dithiophene-benzen (DT-B) with F, which forms an interaction with the thiophene S and gives rise to the F–S type noncovalent conformational locks (NCLs). Single-molecule conductance investigation showed the molecular conductance was increasingly larger with more F substituents. A theoretical study revealed that NCLs play a major role in enhancing the ET rates, which not only led to better π-conjugation but also created additional through-space transport channels. 

Utilizing Noncovalent Conformational Locks to Create Through-Space Charge Transport

Under the dual pressure of energy crisis and environmental pollution, ammonia (NH3) is an indispensable chemical product in the global economy. The electrocatalytic synthesis of NH3 directly from nitrogen (N2) and water (H2O) using renewable electricity has become one of the most attractive and important topics. The basal-plane-activated boron-doped MoS2 nanosheets (B-MoS2) as a non-noble metal catalyst with excellent performance for N2 electroreduction are synthesized by a facile one-step hydrothermal method. In 0.1 M Na2SO4 solution, MoS2 nanosheets doped with 300 mg boric acid (B-MoS2-300) obtain a charming ammonia yield rate of 75.77 µg h-1 mg-1cat. at -0.75 V vs. RHE, and an excellent Faradaic efficiency of 40.11% at -0.60 V vs. RHE. In addition, the B-MoS2-300 nanosheets show good selectivity and chemical stability, and no by-product hydrazine (N2H4) is generated during the reaction. 15N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N2 in the electrolyte. On the one hand, the high conductivity of MoS2 guarantees the electron transfer rate; on the other hand, the successful incorporation of heteroatom B enlarges the interlayer spacing of MoS2, and the B atom can act as an active site for basal plane activation, providing more active sites for NRR. Density functional theory calculation shows that the doping of B activates the base plane of 1T-MoS2, which makes the adsorption of N2 on the base plane easier and promotes the NRR process.

Basal Plane-activated Boron-doped Molybdenum Disulfide Nanosheets for Efficient Electrochemical ammonia synthesis.

To accomplish various complex tasks in the microworld, micro-/nanomotors (MNMs) with diverse swimming characteristics have attracted more and more attention. In this work, ZnO nanoshuttles were synthesized by a simple hydrothermal method. In addition, MNMs based on ZnO nanoshuttles have been designed, exhibiting self-propelled swimming characteristics with three motion modes of shake, rotation, and translation in water. It is revealed that the asymmetrically distributed defects on the surface of ZnO nanoshuttles are responsible for the swimming modes. The unique shuttle-like structure helps to reduce the drag in a low Reynolds number environment and endows the self-propelled ZnO nanoshuttle motor with a relatively high swimming velocity (5.16 μm/s). In addition, to demonstrate the versatility and openness of ZnO nanoshuttle MNMs, ZnO/Co magnetic MNMs and ZnO/TiO2 Janus MNMs were prepared by simple Co doping and TiO2 coating, respectively. This study reveals the possible role of surface defects in regulating the motion behavior of ZnO-based MNMs and also provides a feasible low-cost method for the large-scale fabrication of self-asymmetric fuel-free micro-/nanomotors. 

Self-Propelled Micro-/Nanomotors of ZnO Nanoshuttles Induced by Surface Defects

The advance of single molecular device fabrication strongly relies on the understanding of the metal-molecule-metal junction that can response to the external stimulus. A model Lewis basic molecule DBP which can react with Lewis acid and protic acid was synthesized, then the molecular conducting behavior of the original molecule and the resulted Lewis acid-base pair were researched. Allowing for their identical physical paths for charge conducting, these results indicated that adjusting the molecular electronic structure, even not directly changing the conductive molecular backbone, could also tune the charge transporting ability by nearly one order of magnitude. Furthermore, the addition of another Lewis base - Triethylamine to Lewis acid-base pair brought the electrical properties back to that of single DBP junction, which establishs a basic understanding in the design and construction of reversible and controllable molecular device based on pyridine derived molecule.

Conductance modulation of metal-molecule-metal junction via extra acid addition and its mechanism investigation.

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