The configuration regulation of single‐atom photocatalysts (SAPCs) can significantly influence the interfacial charge transfer and subsequent catalytic process. The construction of conventional SAPCs ...for aqueous CO2 reduction is mainly devoted toward favorable activation and photoreduction of CO2, however, the role of water is frequently neglected. In this work, single Ni atoms are successfully anchored by boron‐oxo species on g‐C3N4 nanosheets through a facile ion‐exchange method. The dative interaction between the B atom and the sp2 N atom of g‐C3N4 guarantees the high dispersion of boron‐oxo species, where O atoms coordinate with single Ni (II) sites to obtain a unique six‐oxygen‐coordinated configuration. The optimized single‐atom Ni photocatalyst, rivaling Pt‐modified g‐C3N4 nanosheets, provides excellent CO2 reduction rate with CO and CH4 as products. Quasi‐in‐situ X‐ray photoelectron spectra, transient absorption spectra, isotopic labeling, and in situ Fourier transform infrared spectra reveal that as‐fabricated six‐oxygen‐coordinated single Ni (II) sites can effectively capture the photoelectrons of CN along the BO bridges and preferentially activate adsorbed water to produce H atoms to eventually induce a hydrogen‐assisted CO2 reduction. This work diversifies the synthetic strategies for single‐atom catalysts and provides insight on correlation between the single‐atom configuration and reaction pathway.
Six‐oxygen‐coordinated single Ni (II) sites are successfully anchored by highly dispersed boron‐oxo species on g‐C3N4 nanosheets. The as‐fabricated single‐atom Ni photocatalyst can realize efficient photocatalytic CO2 reduction, where single Ni atoms can effectively capture photoelectrons and preferentially reduce absorbed water to produce H atoms as active species eventually inducing the reduction of CO2.
The seriousness of the energy crisis and the environmental impact of global anthropogenic activities have led to an urgent need to develop efficient and green fuels. Hydrogen, as a promising ...alternative resource that is produced in an environmentally friendly and sustainable manner by a water splitting reaction, has attracted extensive attention in recent years. However, the large‐scale application of water splitting devices is hindered predominantly by the sluggish oxygen evolution reaction (OER) at the anode. Therefore, the design and exploration of high‐performing OER electrocatalysts is a critical objective. Considering their low prices, abundant reserves, and intrinsic activities, NiFe‐based bimetal compounds are widely studied as excellent OER electrocatalysts. Moreover, recent progress on NiFe‐based OER electrocatalysts in alkaline environments is comprehensively and systematically introduced through various catalyst families including NiFe‐layered hydroxides, metal–organic frameworks, NiFe‐based (oxy)hydroxides, NiFe‐based oxides, NiFe alloys, and NiFe‐based nonoxides. This review briefly introduces the advanced NiFe‐based OER materials and their corresponding reaction mechanisms. Finally, the challenges inherent to and possible strategies for producing extraordinary NiFe‐based electrocatalysts are discussed.
This review briefly introduces the advanced NiFe‐based oxygen evolution reaction (OER) materials and their corresponding reaction mechanisms. After providing this background, recent progress on NiFe‐based OER electrocatalysts through various catalyst families is comprehensively and systematically presented, and the inherent challenges and probable strategies for producing extraordinary NiFe‐based electrocatalysts are finally discussed.
Atomically precise enantiomeric metal clusters are scarce, and copper(I) alkynyl clusters with intense circularly polarized luminescence (CPL) responses have not been reported. A pair of chiral ...alkynyl ligands, (R/S)‐2‐diphenyl‐2‐hydroxylmethylpyrrolidine‐1‐propyne (abbreviated as R/S‐DPM) we successfully prepared and single crystals were characterized of optically pure enantiomeric pair of atomically‐precise copper(I) clusters, Cu14(R/S‐DPM)8(PF6)6 (denoted as R/S‐Cu14), which feature bright red luminescence and CPL with a high luminescence anisotropy factor (glum). A dilute solution containing R/S‐Cu14 was nonluminescent and CPL inactive at room temperature. Crystallization‐ and aggregation‐induced emission (CIE and AIE, respectively) contribute to the triggering of the CPL of R/S‐Cu14 in the crystalline and aggregated states. Their AIE behavior and good biocompatibility indicated applications of these copper(I) clusters in cell imaging in HeLa and NG108‐15 cells.
Atomically precise chiral CuI alkynyl nanoclusters R/S‐Cu14 with inherent chirality were synthesized for the first time. Crystallization‐ and aggregation‐induced emission (CIE and AIE, respectively) trigger circularly polarized luminescence (CPL) with an unprecedented luminescence anisotropy factor (glum).
Heterostructure engineering is an effective technology to improve photo-electronic properties of two dimensional layered semiconductors. In this paper, based on first principles method, we studied ...the structure, stability, energy band, and optical properties of ZnSe/SnSe heterostructure change with film layer. Results show that all heterostructures are the type-II band arrangement, and the interlayer interaction is characterized by van der Waals. The electron concentration and charge density difference implies the electron (holes) transition from SnSe to monolayer ZnSe. By increasing the layer of SnSe films, the quantum effects are weakened leading to the band gap reduced, and eventually show metal properties. The optical properties also have obvious change, the excellent absorption ability of ZnSe/SnSe heterostructures mainly near the infrared spectroscopy. These works suggest that ZnSe/SnSe heterostructure has significant potential for future optoelectronic applications.
The disorderly distribution of defects in the perovskite or at the grain boundaries, surfaces, and interfaces, which seriously affect carrier transport through the formation of nonradiative ...recombination centers, hinders the further improvement on the power conversion efficiency (PCE) of perovskite solar cells (PSCs). Several defect passivation strategies have been confirmed as an efficient approach for promoting the performance of PSCs. Herein, recent progress in the defect passivation toward efficient perovskite solar cells are summarized, and a classification of common passivation strategies that elaborate the mechanism according to the location of the defects and the type of passivation agent is presented. Finally, this review offers likely prospects for future trends in the development of passivation strategies.
Perovskite solar cells still have huge room for improvement in photoelectric conversion efficiency. One of the constraints is the defects at the interface between the perovskite and the transport layer. Passivation is considered a key measure to limit defects. This paper systematically categorizes the effective passivation strategies for perovskites in recent years and gives a future outlook.
Abstract
A class of negative matrices including Vandermonde‐like matrices tends to be extremely ill‐conditioned, and linear systems associated with this class of matrices appear in the polynomial ...interpolation problems. In this article, we present a fast and accurate algorithm with complexity to solve the linear systems whose coefficient matrices belong to the class of negative matrix. We show that the inverse of any such matrix is generated in a subtraction‐free manner. Consequently, the solutions of linear systems associated with the class of negative matrix are accurately determined by parameterization matrices of coefficient matrices, and a pleasantly componentwise forward error is provided to illustrate that each component of the solution is computed to high accuracy. Numerical experiments are performed to confirm the claimed high accuracy.
Chemotherapy has been widely applied in clinics. However, the therapeutic potential of chemotherapy against cancer is seriously dissatisfactory due to the nonspecific drug distribution, multidrug ...resistance (MDR) and the heterogeneity of cancer. Therefore, combinational therapy based on chemotherapy mediated by nanotechnology, has been the trend in clinical research at present, which can result in a remarkably increased therapeutic efficiency with few side effects to normal tissues. Moreover, to achieve the accurate pre-diagnosis and real-time monitoring for tumor, the research of nano-theranostics, which integrates diagnosis with treatment process, is a promising field in cancer treatment. In this review, the recent studies on combinational therapy based on chemotherapy will be systematically discussed. Furthermore, as a current trend in cancer treatment, advance in theranostic nanoparticles based on chemotherapy will be exemplified briefly. Finally, the present challenges and improvement tips will be presented in combination therapy and nano-theranostics.
The vigorous development of green finance has become a national strategy in China. Green finance is gradually becoming a key driver of high-quality economic development and a key area of concern for ...China’s economy and ecological environment. Based on the panel data of 30 Chinese provinces from 2001 to 2019, we analyzed the impact and mechanism of vertical fiscal imbalance (VFI) and green finance (GF) on high-quality economic development (HQD) and then used the fixed-effect model and spatial Durbin model for empirical testing. We found that GF can significantly contribute to HQD, but VFI has a negative moderating effect in contrast to the positive effect of GF on HQD. This negative moderating effect is strongest in the central region. According to the analysis of the spatial econometric model based on geography, economy, and the nested spatial weight matrix, we found that the local GF has a negative spatial transmission effect on the HQD of other regions. Therefore, it is recommended that the coordinated development of green finance among regions be promoted, while affairs and expenditure responsibilities be reasonably distributed between the central and local governments to drive HQD effectively.
Cyber-physical attacks are the main substantial threats facing the utilization and development of the various smart grid technologies. Among these attacks, false data injection attack represents a ...main category with its widely varied types and impacts that have been extensively reported recently. In addressing this threat, several detection algorithms have been developed in the last few years. These were either model-based or data-driven algorithms. This paper provides an intensive summary of these algorithms by categorizing them and elaborating on the pros and cons of each category. The paper starts by introducing the various cyber-physical attacks along with the main reported incidents in history. The significance and the impacts of the false data injection attacks are then reported. The concluding remarks present the main criteria that should be considered in developing future detection algorithms for the false data injection attacks.
Objectives
To develop and validate a radiomics predictive model based on pre-treatment multiparameter magnetic resonance imaging (MRI) features and clinical features to predict a pathological ...complete response (pCR) in patients with locally advanced rectal cancer (LARC) after receiving neoadjuvant chemoradiotherapy (CRT).
Methods
One hundred and eighty-six consecutive patients with LARC (training dataset,
n
= 131; validation dataset,
n
= 55) were enrolled in our retrospective study. A total of 1,188 imaging features were extracted from pre-CRT T2-weighted (T2-w), contrast-enhanced T1-weighted (cT1-w) and ADC images for each patient. Three steps including least absolute shrinkage and selection operator (LASSO) regression were performed to select key features and build a radiomics signature. Combining clinical risk factors, a radiomics nomogram was constructed. The predictive performance was evaluated by receiver operator characteristic (ROC) curve analysis, and then assessed with respect to its calibration, discrimination and clinical usefulness.
Results
Thirty-one of 186 patients (16.7%) achieved pCR. The radiomics signature derived from joint T2-w, ADC, and cT1-w images, comprising 12 selected features, was significantly associated with pCR status and showed better predictive performance than signatures derived from either of them alone in both datasets. The radiomics nomogram, incorporating the radiomics signature and MR-reported T-stages, also showed good discrimination, with areas under the ROC curves (AUCs) of 0.948 (95% CI, 0.907-0.989) and 0.966 (95% CI, 0.924-1.000), as well as good calibration in both datasets. Decision curve analysis confirmed its clinical usefulness.
Conclusions
This study demonstrated that the pre-treatment radiomics nomogram can predict pCR in patients with LARC and potentially guide treatments to select patients for a “wait-and-see” policy.
Key Points
• Radiomics analysis of pre-CRT multiparameter MR images could predict pCR in patients with LARC.
• Proposed radiomics signature from joint T2-w, ADC and cT1-w images showed better predictive performance than individual signatures.
• Most of the clinical characteristics were unable to predict pCR.
PDF
