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.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Crystalline and porous covalent organic frameworks (COFs) and metal‐organic frameworks (MOFs) materials have attracted enormous attention in the field of photocatalytic H2 evolution due to their ...long‐range order structures, large surface areas, outstanding visible light absorbance, and tunable band gaps. In this work, we successfully integrated two‐dimensional (2D) COF with stable MOF. By covalently anchoring NH2‐UiO‐66 onto the surface of TpPa‐1‐COF, a new type of MOF/COF hybrid materials with high surface area, porous framework, and high crystallinity was synthesized. The resulting hierarchical porous hybrid materials show efficient photocatalytic H2 evolution under visible light irradiation. Especially, NH2‐UiO‐66/TpPa‐1‐COF (4:6) exhibits the maximum photocatalytic H2 evolution rate of 23.41 mmol g−1 h−1 (with the TOF of 402.36 h−1), which is approximately 20 times higher than that of the parent TpPa‐1‐COF and the best performance photocatalyst for H2 evolution among various MOF‐ and COF‐based photocatalysts.
Effective separation: A novel MOF/COF hybrid material assembled by covalent connecting two components, exhibits effective visible‐light‐driven photocatalytic H2 evolution due to the ideal band matching and effectively promoting the separation of the photogenerated charges and holes.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Electrocatalysis plays a central role in clean energy conversion, enabling a number of processes for future sustainable technologies. Atomic site electrocatalysts (ASCs), including single-atomic site ...catalysts (SASCs) and diatomic site catalysis (DASCs), are being pursued as economical alternatives to noble-metal-based catalysts for these reactions by virtue of their exceptionally high atom utilization efficiencies, well-defined active sites and high selectivities. In this review, we start from a systematic review on the fabrication routes of ASCs followed by an overview of some new and effective characterization methods to precisely probe the atomic structure. Then we give a comprehensive summary on the current advances in some typical clean energy reactions: water splitting, including hydrogen evolution reaction (HER) and oxygen evolution reaction (OER); oxygen reduction reaction (ORR), including selective 4e
−
- ORR toward H
2
O/OH
−
and 2e
−
- ORR toward H
2
O
2
/HO
2
−
; selective electrooxidation of formic acid, methanol and ethanol (FAOR, MOR and EOR). At the end of this paper, we present a brief conclusion, and discuss the challenges and opportunities on the further development of more selective, active, stable and less expensive ASCs.
This review summarized the fabrication routes and characterization methods of atomic site electrocatalysts (ASCs) followed by their applications for water splitting, oxygen reduction and selective oxidation.
Despite the high long-term survival in localized prostate cancer, metastatic prostate cancer remains largely incurable even after intensive multimodal therapy. The lethality of advanced disease is ...driven by the lack of therapeutic regimens capable of generating durable responses in the setting of extreme tumor heterogeneity on the genetic and cell biological levels. Here, we review available prostate cancer model systems, the prostate cancer genome atlas, cellular and functional heterogeneity in the tumor microenvironment, tumor-intrinsic and tumor-extrinsic mechanisms underlying therapeutic resistance, and technological advances focused on disease detection and management. These advances, along with an improved understanding of the adaptive responses to conventional cancer therapies, anti-androgen therapy, and immunotherapy, are catalyzing development of more effective therapeutic strategies for advanced disease. In particular, knowledge of the heterotypic interactions between and coevolution of cancer and host cells in the tumor microenvironment has illuminated novel therapeutic combinations with a strong potential for more durable therapeutic responses and eventual cures for advanced disease. Improved disease management will also benefit from artificial intelligence-based expert decision support systems for proper standard of care, prognostic determinant biomarkers to minimize overtreatment of localized disease, and new standards of care accelerated by next-generation adaptive clinical trials.
Fused deposition modeling (FDM) is a rapidly growing 3D printing technology. However, printing materials are restricted to acrylonitrile butadiene styrene (ABS) or poly (lactic acid) (PLA) in most ...Fused deposition modeling (FDM) equipment. Here, we report on a new high-performance printing material, polyether-ether-ketone (PEEK), which could surmount these shortcomings. This paper is devoted to studying the influence of layer thickness and raster angle on the mechanical properties of 3D-printed PEEK. Samples with three different layer thicknesses (200, 300 and 400 μm) and raster angles (0°, 30° and 45°) were built using a polyether-ether-ketone (PEEK) 3D printing system and their tensile, compressive and bending strengths were tested. The optimal mechanical properties of polyether-ether-ketone (PEEK) samples were found at a layer thickness of 300 μm and a raster angle of 0°. To evaluate the printing performance of polyether-ether-ketone (PEEK) samples, a comparison was made between the mechanical properties of 3D-printed polyether-ether-ketone (PEEK) and acrylonitrile butadiene styrene (ABS) parts. The results suggest that the average tensile strengths of polyether-ether-ketone (PEEK) parts were 108% higher than those for acrylonitrile butadiene styrene (ABS), and compressive strengths were 114% and bending strengths were 115%. However, the modulus of elasticity for both materials was similar. These results indicate that the mechanical properties of 3D-printed polyether-ether-ketone (PEEK) are superior to 3D-printed ABS.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Big medical data mainly include electronic health record data, medical image data, gene information data, etc. Among them, medical image data account for the vast majority of medical data at this ...stage. How to apply big medical data to clinical practice? This is an issue of great concern to medical and computer researchers, and intelligent imaging and deep learning provide a good answer. This review introduces the application of intelligent imaging and deep learning in the field of big data analysis and early diagnosis of diseases, combining the latest research progress of big data analysis of medical images and the work of our team in the field of big data analysis of medical imagec, especially the classification and segmentation of medical images.
Exosomes, naturally derived nanovesicles secreted from various cell types, can serve as an effective platform for the delivery of various cargoes, because of their intrinsic ability such as long ...blood circulation and immune escapinge. However, unlike conventional synthetic nanoparticles, drug release from exosomes at defined targets is not controllable. Moreover, endowing exosomes with satisfactory cancer‐targeting ability is highly challenging. Here, for the first time, a biological and synthetic hybrid designer exosome is described with photoresponsive functionalities based on a donor cell‐assisted membrane modification strategy. Practically, the designer exosome effectively accumulates at target tumor sites via dual ligand‐mediated endocytosis. Then the localized hyperthermia induced by the conjunct gold nanorods under near‐infrared irradiation impacts the permeability of exosome membrane to enhance drug release from exosomes, thus inhibiting tumor relapse in a programmable manner. The designer exosome combines the merits of both synthetic materials and the natural nanovesicles. It not only preserves the intrinsic functionalities of native exosome, but also gains multiple abilities for efficient tumor targeting, controlled release, and thermal therapy like synthetic nanocarriers. The versatile designer exosome can provide functional platforms by engineering with more multifarious functionalities from synthetic materials to achieve individualized precise cancer therapy in the future.
A biological and synthetic hybrid designer exosome is presented with photoresponsive functionalities based on a donor cell‐assisted membrane modification strategy. The dual ligand engineered exosomes are shown to significantly increase accumulation at the target tumor site and can burst release drug under controllable near‐infrared irradiation in vitro and in vivo.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this ...work, we firstly realized overall water splitting activity of β-ketoamine COFs by systematically engineering N-sites, architecture, and morphology. By in situ incorporating sub-nanometer platinum (Pt) nanoparticles co-catalyst into the pores of COFs nanosheets, both Pt@TpBpy-NS and Pt@TpBpy-2-NS show visible-light-driven overall water splitting activity, with the optimal H
and O
evolution activities of 9.9 and 4.8 μmol in 5 h for Pt@TpBpy-NS, respectively, and a maximum solar-to-hydrogen efficiency of 0.23%. The crucial factors affecting the activity including N-sites position, nano morphology, and co-catalyst distribution were systematically explored. Further mechanism investigation reveals the tiny diversity of N sites in COFs that induces great differences in electron transfer as well as reaction potential barriers.
Engineering, controlling, and simulating quantum dynamics is a strenuous task. However, these techniques are crucial to develop quantum technologies, preserve quantum properties, and engineer ...decoherence. Earlier results have demonstrated reservoir engineering, construction of a quantum simulator for Markovian open systems, and controlled transition from Markovian to non-Markovian regime. Dephasing is an ubiquitous mechanism to degrade the performance of quantum computers. However, all-purpose quantum simulator for generic dephasing is still missing. Here, we demonstrate full experimental control of dephasing allowing us to implement arbitrary decoherence dynamics of a qubit. As examples, we use a photon to simulate the dynamics of a qubit coupled to an Ising chain in a transverse field and also demonstrate a simulation of nonpositive dynamical map. Our platform opens the possibility to simulate dephasing of any physical system and study fundamental questions on open quantum systems.
In this work, we have developed a mild route to fabricate typically mesoporous Mo2C-C hybrid nanospheres based on a solvothermal synthesis and reduction-carbonization process. This work opens a ...low-temperature route to synthesize valuable carbides. The resultant Mo2C-C hybrid, for the first time, is used as an anode material in lithium ion batteries (LIBs). Compared with bulk Mo2C, the Mo2C-C hybrid exhibits much better electrochemical performance. Remarkably, the hybrid electrode can deliver a specific capacity of over 670 mA h g(-1) after 50 cycles at 100 mA g(-1), which is much higher than that of the bulk material (113 mA h g(-1)). Even cycled at a high current density of 1000 mA g(-1), high capacities of around 400-470 mA h g(-1) can still be retained for the Mo2C-C hybrid. It might benefit from the synergistic effect of the nanohybridization, effectively relieving the volume change during the repeated lithium insertion-extraction reactions and maintaining the integrity of the electrical connections. It is expected that the present synthesis strategy for the Mo2C-C hybrid can be extended to other nanostructured carbides with good energy storage performance.
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