Role and prospects of green quantum dots in photoelectrochemical hydrogen generation: A review

Eco-friendly quantum dots (QDs) can be termed green QDs which stand as an attractive choice to modify the properties of known semiconductors in the direction of getting efficient photoelectrodes for solar-induced photoelectrochemical (PEC) splitting of water, due to their peculiar properties. Thus, it is of high significance to analyze their merit/demerit as an effective scaffold in PEC cell. QDs are known for their excellent optical properties however, the coupling of green QDs with semiconductor is not only useful in improving absorption characteristics but also promotes charge transfer. This review has undertaken the critical analysis on the worldwide research going on the green QDs modified photoelectrode with respect to their optical, electrical & photoelectrochemical properties, role, usefulness, efficiency, and finally the success in PEC system for hydrogen production. Various methods on the facile synthesis & sensitization techniques of green QDs available in the literature have also been discussed. Further, recent advances on the development of green QDs based photo-electrode, along with major challenges of using green QDs in this field have also been presented.     

Role of functionalized graphene quantum dots in hydrogen evolution reaction: A density functional theory study

Rapid advances in the field of catalysis require a microscopic understanding of the catalytic mechanisms. However, in recent times, experimental insights in this field have fallen short of expectations. Furthermore, experimental searches of novel catalytic materials are expensive and time-consuming, with no guarantees of success. As a result, density functional theory (DFT) can be quite advantageous in advancing this field because of the microscopic insights it provides and thus can guide experimental searches of novel catalysts. Several recent works have demonstrated that low-dimensional materials can be very efficient catalysts. Graphene quantum dots (GQDs) have gained much attention in past years due to their unique properties like low toxicity, chemical inertness, biocompatibility, crystallinity, etc. These properties of GQDs which are due to quantum confinement and edge effects facilitate their applications in various fields like sensing, photoelectronics, catalysis, and many more. Furthermore, the properties of GQDs can be enhanced by doping and functionalization. In order to understand the effects of functionalization by oxygen and boron based groups on the catalytic properties relevant to the hydrogen-evolution reaction (HER), we perform a systematic study of GQDs functionalized with the oxygen (O), borinic acid (BC₂O), and boronic acid (BCO₂). All calculations that included geometry optimization, electronic and adsorption mechanism, were carried out using the Gaussian16 package, employing the hybrid functional B3LYP, and the basis set 6-31G(d,p). With the variation in functionalization groups in GQDs, we observe significant changes in their electronic properties. The adsorption energy E_ads of hydrogen over O-GQD, BC₂O-GQD, and BCO₂-GQD is ?0.059 eV, ?0.031 eV and ?0.032 eV respectively. Accordingly, Gibbs free energy (ΔG) of hydrogen adsorption is extraordinarily near the ideal value (0 eV) for all the three types of functionalized GQDs. Thus, the present work suggests pathways for experimental realization of low-cost and multifunctional GQDs based catalysts for clean and renewable hydrogen energy production.     

Concentration dependence of physical properties of low temperature processed ZnO quantum dots thin films on polyethylene terephthalate as potential electron transport material for perovskite solar cell

Colloidal Zinc oxide quantum dots (ZnO QDs) prepared with varying concentrations through precipitation method were deposited on flexible ITO/PET substrates using spin-coating technique. Various characterization tools were utilized to investigate the morphological, structural, electrical and optical properties of the films. The crystallinity of the films was found to improve with increasing ZnO QD concentration (ZQ_C) as evident from the X-ray diffraction (XRD) and field emission scanning electron microscopy (FE-SEM) studies. Crystallographic and optical parameters were evaluated and explained in depth. The average nanograin size and bandgap were increased and decreased respectively, from ～5 nm to ～8 nm and 3.29 eV–3.24 eV with an increase in ZQ_C from 10 mg/mL to 70 mg/mL. Columnar structure growth of the films is revealed by AFM results. The films showed decent optical transparency up to 81%. All the ZnO films exhibited n-type semiconducting property as indicated by the electrical measurements with carrier mobility and low resistivity of 12.21–26.63 cm²/Vs and 11.84 × 10^?3 to 13.16 × 10^?3 Ω cm respectively. Based on the experimental findings, ZnO QD nanostructure film grown at 50 mg/mL is envisaged to be a potential candidate for flexible perovskite photovoltaic application.     

基于Matlab的量子激光雷达稳频通信模拟系统设计

传统通信模拟系统设计较为复杂,导致模拟过程消耗能量较大,不能准确模拟稳频通信质量。因此,提出基于Matlab的量子激光雷达稳频通信模拟系统。由于振荡器是雷达形成初始信号源的基础,通过分析振荡电路与相位噪声,获得相位噪声函数与通信频率存在的关系;为确保通信过程的稳定,将准确性与稳定性作为信号质量的评价指标,并采用锁频环稳频技术计算频率偏移程度,根据PID控制算法控制频率,量子激光雷达稳频通信;利用Matlab确定激光器、探测器等硬件组成结构,通过时序与数字阵列的设置完成模拟系统设计。仿真结果表明所提系统结构简便、性能稳定,能够真实模拟出稳频通信的信号质量。     

Superconducting Quantum Metamaterials from High Pressure Melt Infiltration of Metals into Block Copolymer Double Gyroid Derived Ceramic Templates

Mesoscale order can lead to emergent properties including phononic bandgaps or topologically protected states. Block copolymers offer a route to mesoscale periodic architectures, but their use as structure directing agents for metallic materials has not been fully realized. A versatile approach to mesostructured metals via bulk block copolymer self-assembly derived ceramic templates, is demonstrated. Molten indium is infiltrated into mesoporous, double gyroidal silicon nitride templates under high pressure to yield bulk, 3D periodic nanocomposites as free-standing monoliths which exhibit emergent quantum-scale phenomena. Vortices are artificially introduced when double gyroidal indium metal behaves as a type II superconductor, with evidence of strong pinning centers arrayed on the order of the double gyroid lattice size. Sample behavior is reproducible over months, showing high stability. High pressure infiltration of bulk block copolymer self-assembly based ceramic templates is an enabling tool for studying high-quality metals with previously inaccessible architectures, and paves the way for the emerging field of block-copolymer derived quantum metamaterials.     

Construction of CaTiO3 nanosheets with boron nitride quantum dots as effective photogenerated hole extractor for boosting photocatalytic performance under simulated sunlight

Herein, titanate-based perovskite CaTiO₃ nanosheets were successfully designed via boron nitride quantum dots (BNQDs) to fabricate CaTiO₃/BNQDs catalyst. The as-fabricated composite catalysts were analysed by transmission electron microscope (TEM), scanning electron microscopy coupled with energy dispersive spectrometry (SEM-EDS), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR), X-ray diffraction (XRD), UV–vis spectroscopy (UV-DRS), photoluminescence (PL) and electrochemical impedance spectroscopy (EIS) techniques. SEM-Mapping analysis showed that the boron and nitrogen elements dispersed well over the CaTiO₃ surface which was useful for building electronic channels for rapid transport of photo-induced charge pairs. TEM images verified the attachment of BNQDs around the surface of host CaTiO₃ forming intimate interface while the distribution of chemical states was observed by XPS analysis demonstrating strong coupling effect between BNQDs and CaTiO₃ through Ti–O–N and Ti–O–B bonds. Moreover, PL and light absorption properties enhanced with the quantum confinement effect of BNQDs. As expected, the photocatalytic degradation rate of CaTiO₃/BNQDs was increased to k_app = 0.015 min^{? 1} with optimum BNQDs loading, which was 2.31 times folder than that of bare CaTiO₃ (0.006 min^{? 1}). The enhanced photocatalytic efficiency was observed for CaTiO₃/BNQDs than pristine perovskite on account of formation of electron tapping sites, decreased band gap energy and hindered recombination rate. On the other hand, in the presence of H₂O₂, the degradation percentage increased from 88.5% to 92.1% at the end of 120 min of irradiation while 96.8% of TC was quickly degraded within 60 min after activating with peroxymonosulfate which created strong sulphate radicals. Radical trapping tests indicated that the photo-generated holes were the primary active species in the photocatalytic mechanism. Moreover, CaTiO₃/BNQDs catalyst showed excellent stability in recycling tests. Besides, the possible degradation mechanism was proposed. This study shed light on the significance of BNQDs in the enhancement of the photocatalytic activities of titanate-based perovskite for effective degradation of tetracycline antibiotic in contaminated water.     

Machine learning of phases and mechanical properties in complex concentrated alloys

The mechanical properties of complex concentrated alloys (CCAs) depend on their formed phases and corresponding microstructures.The data-driven prediction of the phase formation and associated mechanical properties is essential to discovering novel CCAs.The present work collects 557 samples of various chemical compositions,comprising 61 amorphous,167 single-phase crystalline,and 329 multi-phases crystalline CCAs.Three classification models are developed with high accuracies to category and understand the formed phases of CCAs.Also,two regression models are constructed to predict the hard-ness and ultimate tensile strength of CCAs,and the correlation coefficient of the random forest regression model is greater than 0.9 for both of two targeted properties.Furthermore,the Shapley additive expla-nation (SHAP) values are calculated,and accordingly four most important features are identified.A significant finding in the SHAP values is that there exists a critical value in each of the top four fea-tures,which provides an easy and fast assessment in the design of improved mechanical properties of CCAs.The present work demonstrates the great potential of machine learning in the design of advanced CCAs.     

锡量子点制备及其电催化还原二氧化碳产甲酸性能

锡基材料在自然界含量丰富、价格低廉, 在电催化还原CO₂制液体燃料反应中具有巨大潜力。但是较低的产物选择性和较差的稳定性限制了其应用。本工作制备的锡量子点电催化剂(Sn-QDs), 具有高效、高稳定性和高选择性的电催化还原CO₂产HCOOH活性。Sn-QDs的平均颗粒尺寸仅为2~3 nm, 结晶性良好。小的颗粒尺寸增大了电化学活性面积(ECSA), Sn-QDs的ECSA约为锡颗粒的4.4倍。ECSA增大以及CO₂还原反应动力学加速, 促进了CO₂电化学转化。在-1.0 V (vs RHE)下, Sn-QDs/CN催化剂的HCOOH法拉第效率(FE_HCOOH)达到95%, 并且在宽约0.5 V的电势范围内能够保持在83%以上。此外, Sn-QDs/CN可以在24 h内保持良好的电化学稳定性。     

Matrix Manipulation of Directly-Synthesized PbS Quantum Dot Inks Enabled by Coordination Engineering

The direct-synthesis of conductive PbS quantum dot (QD) ink is facile, scalable, and low-cost, boosting the future commercialization of optoelectronics based on colloidal QDs. However, manipulating the QD matrix structures still is a challenge, which limits the corresponding QD solar cell performance. Here, for the first time a coordination-engineering strategy to finely adjust the matrix thickness around the QDs is presented, in which halogen salts are introduced into the reaction to convert the excessive insulating lead iodide into soluble iodoplumbate species. As a result, the obtained QD film exhibits shrunk insulating shells, leading to higher charge carrier transport and superior surface passivation compared to the control devices. A significantly improved power-conversion efficiency from 10.52% to 12.12% can be achieved after the matrix engineering. Therefore, the work shows high significance in promoting the practical application of directly synthesized PbS QD inks in large-area low-cost optoelectronic devices.     

以任意高维纠缠态为量子信道的受控隐形传态

目的是利用高维量子纠缠态为量子信道，讨论未知单粒子态的受控隐形传输问题。以三维量子纠缠态为信道，提出一个二维任意单粒子态的受控隐形传输协议。提出了以任意[d]-维量子纠缠态为量子信道，[t]-维任意单粒子态的隐形传输协议[(t相似文献