Engineering grain boundaries at the 2D limit for the hydrogen evolution reaction

Atom-thin transition metal dichalcogenides (TMDs) have emerged as fascinating materials and key structures for electrocatalysis. So far, their edges, dopant heteroatoms and defects have been intensively explored as active sites for the hydrogen evolution reaction (HER) to split water. However, grain boundaries (GBs), a key type of defects in TMDs, have been overlooked due to their low density and large structural variations. Here, we demonstrate the synthesis of wafer-size atom-thin TMD films with an ultra-high-density of GBs, up to ~1012 cm−2. We propose a climb and drive 0D/2D interaction to explain the underlying growth mechanism. The electrocatalytic activity of the nanograin film is comprehensively examined by micro-electrochemical measurements, showing an excellent hydrogen-evolution performance (onset potential: −25 mV and Tafel slope: 54 mV dec−1), thus indicating an intrinsically high activation of the TMD GBs

Identification of Radioactive Mineralized Lithology and Mineral Prospectivity Mapping Based on Remote Sensing in High-Latitude Regions: A Case Study on the Narsaq Region of Greenland

The harsh environment of high-latitude areas with large amounts of snow and ice cover makes it difficult to carry out full geological field surveys. Uranium resources are abundant within the Ilimaussaq Complex in the Narsaq region of Greenland, where the uranium ore body is strictly controlled by the Lujavrite formation, which is the main ore-bearing rock in the complex rock mass. Further, large aggregations of radioactive minerals appear as thermal anomalies on remote sensing thermal infrared imagery, which is indicative of deposits of highly radioactive elements. Using a weight-of-evidence analysis method that combines machine-learned lithological classification information with information on surface temperature thermal anomalies, the prediction of radioactive element-bearing deposits at high latitudes was carried out. Through the use of Worldview-2 (WV-2) remote sensing images, support vector machine algorithms based on texture features and topographic features were used to identify Lujavrite. In addition, the distribution of thermal anomalies associated with radioactive elements was inverted using Landsat 8 TIRS thermal infrared data. From the results, it was found that the overall accuracy of the SVM algorithm-based lithology mapping was 89.57%. The surface temperature thermal anomaly had a Spearman correlation coefficient of 0.63 with the total airborne measured uranium gamma radiation. The lithological classification information was integrated with surface temperature thermal anomalies and other multi-source remote sensing mineralization elements to calculate mineralization-favorable areas through a weight-of-evidence model, with high-value mineralization probability areas being spatially consistent with known mineralization areas. In conclusion, a multifaceted remote sensing information finding method, focusing on surface temperature thermal anomalies in high-latitude areas, provides guidance and has reference value for the exploration of potential mineralization areas for deposits containing radioactive elements

Interface Engineering To Boost Photoresponse Performance of Self-Powered, Broad-Bandwidth PEDOT:PSS/Si Heterojunction Photodetector

Organic–inorganic hybrid heterojunctions are poised to push toward novel optoelectronics applications, such as photodetectors, but significant challenges complicating practical use remain. Although all organic based photodetectors have been reported with great success, their potential in high-speed, broadband, self-powered photodetectors have not been fully explored. Herein, a self-powered, broad bandwidth of photodetector based on PEDOT:PSS/Si heterojunction is built by a facial low temperature spin-coating method. By interface engineering of heterojunction with optimal band alignment and heteromicrostructures, enhanced photoresponse performances are obtained. The bandwidth of the hybrid photodetector could be broadened by 10 kHz after interfacial passivation by a methyl group. Further manipulating the geometrical structure of the hybrid heterojunction with silicon nanowire, a broad spectrum response from 300 to 1100 nm, with bandwidth as high as 40.6 kHz, fast response speed of 2.03 μs and high detection of 4.1 × 10¹¹ Jones under zero bias was achieved. Meanwhile, the close dependence between the photoresponse performance of heterojunctions and Si nanowire length is observed in the top-coverage configuration. Finally, a coverage effects model is proposed based on the competition of Si bulk and surface recombination, which is also confirmed by the designed bottom-coverage experiment. The mechanisms behind the enhanced photoresponse of the hybrid photodetector is attributed to the optimum band alignment, as well as the optimum balance of carrier dissociation and recombination of heterojunction. The scalable and low temperature method would be of great convenience for large-scale fabrication of the PEDOT:PSS/Si hybrid photodetector

Rational Engineering of 2D Materials as Advanced Catalyst Cathodes for High‐Performance Metal–Carbon Dioxide Batteries

Given the unique characteristic of integrating CO2 conversion and renewable energy storage, metal–CO2 batteries (MCBs) are expected to become the next‐generation technology to address both environmental and energy crises. As involving complex gas–liquid–solid three‐phase interfacial reactions, cathodes of MCBs can significantly affect the overall battery operation, thus attracting much research attention. Compared to conventional materials, 2D materials offer great opportunities for the design and preparation of high‐performance catalyst cathodes, especially showing superior bifunctional electrocatalytic capacity for rechargeable MCBs. The inherent high‐specific‐surface area and diverse structural architectures of 2D materials enable their flexible and rational engineering designs toward kinetically favorable metal–CO2 electrochemistry. Herein this review, the cutting‐edge progresses of 2D materials‐based catalyst cathodes are presented in MCBs. The reaction mechanisms of various MCBs, including both nonaqueous and aqueous systems, are systematically introduced. Then, the design criteria of catalyst cathodes, and the merits and demerits of 2D materials‐based catalyst cathodes are discussed. After that, three representative engineering strategies (i.e., defect control, phase engineering, and heterostructure design) of 2D materials for high‐performance MCBs are systematically described. Finally, the current research advances are briefly summarized and the confronting challenges and opportunities for future development of advanced MCB cathodes are proposed

Facet-Dependent Property of Sequentially Deposited Perovskite Thin Films: Chemical Origin and Self-Annihilation

Quantification of intergrain length scale properties of CH₃NH₃PbI₃ (MAPbI₃) can provide further understanding of material physics, leading to improved device performance. In this work, we noticed that two typical types of facets appear in sequential deposited perovskite (SDP) films: smooth and steplike morphologies. By mapping the surface potential as well as the photoluminescence (PL) peak position, we revealed the heterogeneity of SDP thin films that smooth facets are almost intrinsic with a PL peak at 775 nm, while the steplike facets are <i>p</i>-type-doped with 5-nm blue-shifted PL peak. Considering the reaction process, we propose that the smooth facets have well-defined crystal lattices that resulted from the interfacial reaction between MAI and PbI₂ domains containing low trap states density. The steplike facets are MAI-rich originated from the grain boundaries of PbI₂ film and own more trap states. Conversion of steplike facets to smooth facets can be controlled by increasing the reaction time through Ostwald ripening. The improved stability, photoresponsivity up to 0.3 A/W, on/off ratio up to 3900, and decreased photo response time to ∼160 μs show that the trap states can be annihilated effectively to improve the photoelectrical conversion with prolonged reaction time and elimination of steplike facets. Our findings demonstrate the relationship between the facet heterogeneity of SDP films and crystal growth process for the first time, and imply that the systematic control of crystal grain modification will enable amelioration of crystallinity for more-efficient perovskite photoelectrical applications