Photoreduction of N₂ is among the most interesting and challenging methods for N₂ fixation under mild conditions. In this study, we determined that nitrogen vacancies (NVs) could endow graphitic carbon nitride (g-C₃N₄) with the photocatalytic N₂ fixation ability. Photocatalytic N₂ fixation induced by NVs is free from the interference of other gases. The reason is that NVs could selectively adsorb and activate N₂ because NVs have the same shape and size as the nitrogen atom in N₂. In addition to this, NVs could also improve many other properties of g-C₃N₄ to support photocatalytic N₂ fixation. These new findings could elucidate the design of efficient photocatalysts for photocatalytic N₂ fixation.

Selective photocatalytic N₂ fixation dependent on g-C₃N₄ induced by nitrogen vacancies

Simultaneously Realizing Rapid Electron Transfer and Mass Transport in Jellyfish-Like Mott–Schottky Nanoreactors for Oxygen Reduction Reaction

The functions of interfacial synergy in heterojunction catalysts are diverse and powerful, providing a route to solve many difficulties in energy conversion and organic synthesis. Among heterojunction-based catalysts, the Mott-Schottky catalysts composed of a metal-semiconductor heterojunction with predictable and designable interfacial synergy are rising stars of next-generation catalysts. We review the concept of Mott-Schottky catalysts and discuss their applications in various realms of catalysis. In particular, the design of a Mott-Schottky catalyst provides a feasible strategy to boost energy conversion and chemical synthesis processes, even allowing realization of novel catalytic functions such as enhanced redox activity, Lewis acid-base pairs, and electron donor-acceptor couples for dealing with the current problems in catalysis for energy conversion and storage. This review focuses on the synthesis, assembly, and characterization of Schottky heterojunctions for photocatalysis, electrocatalysis, and organic synthesis. The proposed design principles, including the importance of constructing stable and clean interfaces, tuning work function differences, and preparing exposable interfacial structures for designing electronic interfaces, will provide a reference for the development of all heterojunction-type catalysts, electrodes, energy conversion/storage devices, and even super absorbers, which are currently topics of interest in fields such as electrocatalysis, fuel cells, CO2 reduction, and wastewater treatment.

Design of the Synergistic Rectifying Interfaces in Mott-Schottky Catalysts.

Engineering of defects in semiconductors provides an effective protocol for improving photocatalytic N2 conversion efficiency. This review focuses on the state-of-the-art progress in defect engineering of photocatalysts for the N2 reduction toward ammonia. The basic principles and mechanisms of thermal catalyzed and photon-induced N2 reduction are first concisely recapped, including relevant properties of the N2 molecule, reaction pathways, and NH3 quantification methods. Subsequently, defect classification, synthesis strategies, and identification techniques are compendiously summarized. Advances of in situ characterization techniques for monitoring defect state during the N2 reduction process are also described. Especially, various surface defect strategies and their critical roles in improving the N2 photoreduction performance are highlighted, including surface vacancies (i.e., anionic vacancies and cationic vacancies), heteroatom doping (i.e., metal element doping and nonmetal element doping), and atomically defined surface sites. Finally, future opportunities and challenges as well as perspectives on further development of defect-engineered photocatalysts for the nitrogen reduction to ammonia are presented. It is expected that this review can provide a profound guidance for more specialized design of defect-engineered catalysts with high activity and stability for nitrogen photochemical fixation.

/pdf/photocatalytic-nitrogen-reduction-to-ammonia-insights-into-4bbb0mjemq.pdf

Photocatalytic nitrogen reduction to ammonia: Insights into the role of defect engineering in photocatalysts

Solar-powered N2 reduction in aqueous solution is becoming a research hotspot for ammonia production. Schottky junctions at the metal/semiconductor interface have been effective to build up a one-way channel for the delivery of photogenerated electrons toward photoredox reactions. However, their applications for enhancing the aqueous phase reduction of N2 to ammonia have been bottlenecked by the difficulty of N2 activation and the competing H2 evolution reaction (HER) at the metal surface. Herein, the application of Bi with low HER activity as a robust cocatalyst for constructing Schottky-junction photocatalysts toward N2 reduction to ammonia is reported. The introduction of Bi not only boosts the interfacial electron transfer from excited photocatalysts due to the built-in Schottky-junction effect at the Bi/semiconductor interface but also synchronously facilitates the on-site N2 adsorption and activation toward solar ammonia production. The unidirectional charge transfer to the active site of Bi significantly promotes the photocatalytic N2-to-ammonia conversion efficiency by 65 times for BiOBr. In addition, utilizing Bi to enhance the photocatalytic ammonia production can be extended to other semiconductor systems. This work is expected to unlock the promise of engineering Schottky junctions toward high-efficiency solar N2-to-ammonia conversion in aqueous phase.

https://www.onlinelibrary.wiley.com/doi/pdf/10.1002/advs.202003626

Schottky Junctions with Bi Cocatalyst for Taming Aqueous Phase N 2 Reduction toward Enhanced Solar Ammonia Production.

Electronic control of Fe nanoparticles can provide a great opportunity to manipulate their magnetic properties and improve their catalytic activity. Herein, superparamagnetic Fe nanoclusters with Pt2+ doping are synthesized on a variety of semiconductor nitrides, oxides and silicon. Compared to the intrinsic Fe nanoclusters, the as-synthesized Pt-doped Fe nanoclusters exhibit ultrasmall size with a very low saturation magnetization (2.0 emu g−1) and high electron delocalization. The incorporation of Pt2+ dopants also leads to the successful formation of a large Schottky barrier at the iron/semiconductor interface and renders semiconductor a powerful electron donor for Fe active sites under photo irradiation. Photoluminescence spectroscopy and transient photocurrent responses indicate that the formed Schottky barrier can significantly promote the separation of photogenerated charge carriers. Mott-Schottky photocatalysts with enhanced back donation ability provides an efficient pathway to promote N N bond cleavage and produce ammonia with H2 at room temperature by visible light.

Fe-Pt nanoclusters modified Mott-Schottky photocatalysts for enhanced ammonia synthesis at ambient conditions

High-precision real-time UAV target recognition based on improved YOLOv4

Introduction Mutation patterns have been extensively explored to decipher the etiologies of hepatocellular carcinoma (HCC). However, the study and potential clinical role of mutation patterns to stratify high-risk patients and optimize precision therapeutic strategies remain elusive in HCC. Methods Using exon-sequencing data in public (n=362) and in-house (n=30) cohorts, mutation signatures were extracted to decipher relationships with the etiology and prognosis in HCC. The proteomics (n=159) and cell-line transcriptome data (n=1019) were collected to screen the implication of sensitive drugs. A novel multi-step machine-learning framework was then performed to construct a classification predictor, including recognizing stable reversed gene pairs, establishing a robust prediction model, and validating the robustness of the predictor in five independent cohorts (n=900). Results Two heterogeneous mutation signature clusters were identified, and a high-risk prognosis cluster was recognized for further analysis. Notably, mutation signature cluster 1 (MSC1) was featured by activated anti-tumor immune and metabolism dysfunctional states, higher genomic instability (high TMB, SNV neoantigen, indel neoantigens, and total neoantigens), and a dismal prognosis. Notably, MSC performed as an independent risk factor than clinical traits (eg, stage, vascular invasion). Additionally, afatinib and canertinib were recognized which might have potential therapeutic implications in MSC1, and the targets of these drugs presented a higher expression in both gene and protein levels in HCC. Discussion Our studies may provide a promising platform for improving prognosis and tailoring therapy in HCC.

https://www.dovepress.com/getfile.php?fileID=87505

Prognosis and Personalized Treatment Prediction in Different Mutation-Signature Hepatocellular Carcinoma

To facilitate ground station monitoring and command uploading, unmanned aerial vehicles (UAVs) need to frequently exchange individual state data between units. However, this results in a significant usage of communication bandwidth. To address this issue, on the basis of an event-triggered strategy, this paper proposes an Extended Kalman Filter (EKF). aimed at reducing the communication burden of UAVs while maintaining high accuracy. Specifically, a state measurement triggered by an event is selected for filtering only if it contains innovation, thereby reducing the amount of data that needs to be communicated. Since UAV systems are nonlinear, EKF is adopted to fully utilize the information obtained from event-triggered strategies, thereby enhancing the estimation performance. In this paper, a physical UAV was used to verify the proposed algorithm, and it proved to have robust dynamic performance and to effectively reduce the communication rate.

Event-triggered Extended Kalman Filter for UAV Monitoring System

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Fe-Pt nanoclusters modified Mott-Schottky photocatalysts for enhanced ammonia synthesis at ambient conditions

High-precision real-time UAV target recognition based on improved YOLOv4

Prognosis and Personalized Treatment Prediction in Different Mutation-Signature Hepatocellular Carcinoma

Event-triggered Extended Kalman Filter for UAV Monitoring System