The conversion of solar energy to chemical energy is a promising way of generating renewable energy. Hydrogen production by means of water splitting over semiconductor photocatalysts is a simple, ...cost-effective approach to large-scale solar hydrogen synthesis. Since the discovery of the Honda–Fujishima effect, considerable progress has been made in this field, and numerous photocatalytic materials and water-splitting systems have been developed. In this Review, we summarize existing water-splitting systems based on particulate photocatalysts, focusing on the main components: light-harvesting semiconductors and co-catalysts. The essential design principles of the materials employed for overall water-splitting systems based on one-step and two-step photoexcitation are also discussed, concentrating on three elementary processes: photoabsorption, charge transfer and surface catalytic reactions. Finally, we outline challenges and potential advances associated with solar water splitting by particulate photocatalysts for future commercial applications.Overall water splitting using powdered photocatalysts is a promising approach to large-scale solar hydrogen production. This Review details recent developments in particulate photocatalysts for overall water splitting based on one- and two-step photoexcitation systems.
The spraying method is developed for the fabrication of mechanically robust and self‐healing superhydrophobic coatings, which comprise highly porous and rough polyelectrolyte coatings preserved with ...low‐surface‐energy healing agents. These coatings can repetitively and autonomically restore superhydrophobicity in humid environments. After depletion of healing agents, superhydrophobic coatings with dual healing agents can regain their self‐healing ability by re‐spraying fluoroalkylsilane.
After decades of evolution, measuring instruments for quantitative gait analysis have become an important clinical tool for assessing pathologies manifested by gait abnormalities. However, such ...instruments tend to be expensive and require expert operation and maintenance besides their high cost, thus limiting them to only a small number of specialized centers. Consequently, gait analysis in most clinics today still relies on observation-based assessment. Recent advances in wearable sensors, especially inertial body sensors, have opened up a promising future for gait analysis. Not only can these sensors be more easily adopted in clinical diagnosis and treatment procedures than their current counterparts, but they can also monitor gait continuously outside clinics - hence providing seamless patient analysis from clinics to free-living environments. The purpose of this paper is to provide a systematic review of current techniques for quantitative gait analysis and to propose key metrics for evaluating both existing and emerging methods for qualifying the gait features extracted from wearable sensors. It aims to highlight key advances in this rapidly evolving research field and outline potential future directions for both research and clinical applications.
A novel stimuli‐responsive hydrogel system with liposomes serving as both noncovalent crosslinkers and functional small molecules carriers for controlled‐release is developed. Liposomes can crosslink ...polyacrylamide copolymers functionalized with cholesterol‐modified DNA motifs to yield a DNA hydrogel system, due to the hydrophobic interaction between cholesteryl groups and the lipid bilayer of liposomes. Functional information encoded DNA motifs on the polymer backbones endow the hydrogel with programmable smart responsive properties. In a model system, the hydrogel exhibits stimuli‐responsive gel‐to‐sol transformation triggered by the opening of DNA motifs upon the presence of a restriction endonuclease enzyme, EcoR I, or temperature change, realizing the controlled‐release of liposomes which are highly efficient carriers of active small molecules payloads. Two active molecules, 1,1‐dioctadecyl‐3,3,3,3‐tetramethylindodicarbocyanine perchlorate (DiIC18(5)) and calcein, are chosen as the hydrophobic and hydrophilic model payloads, respectively, to address the feasibility of the releasing strategy. Moreover, the hydrogel exhibits injectable property as well as self‐recovery behaviors.
A stimuli‐responsive liposome crosslinked DNA hydrogel is developed with liposomes serving as both the noncovalent crosslinkers and microcarriers of hydrophilic or hydrophobic functional small molecule payloads. Controlled‐release is triggered via either enzyme or raising the temperature. Besides, the hydrogel shows thermoreversible behavior and injectable property as well as self‐recovery ability.
Low bandgap n-type organic semiconductor (n-OS) ITIC has attracted great attention for the application as an acceptor with medium bandgap p-type conjugated polymer as donor in nonfullerene polymer ...solar cells (PSCs) because of its attractive photovoltaic performance. Here we report a modification on the molecular structure of ITIC by side-chain isomerization with meta-alkyl-phenyl substitution, m-ITIC, to further improve its photovoltaic performance. In a comparison with its isomeric counterpart ITIC with para-alkyl-phenyl substitution, m-ITIC shows a higher film absorption coefficient, a larger crystalline coherence, and higher electron mobility. These inherent advantages of m-ITIC resulted in a higher power conversion efficiency (PCE) of 11.77% for the nonfullerene PSCs with m-ITIC as acceptor and a medium bandgap polymer J61 as donor, which is significantly improved over that (10.57%) of the corresponding devices with ITIC as acceptor. To the best of our knowledge, the PCE of 11.77% is one of the highest values reported in the literature to date for nonfullerene PSCs. More importantly, the m-ITIC-based device shows less thickness-dependent photovoltaic behavior than ITIC-based devices in the active-layer thickness range of 80–360 nm, which is beneficial for large area device fabrication. These results indicate that m-ITIC is a promising low bandgap n-OS for the application as an acceptor in PSCs, and the side-chain isomerization could be an easy and convenient way to further improve the photovoltaic performance of the donor and acceptor materials for high efficiency PSCs.
Chimeric antigen receptor T (CAR-T) cell therapy represents a major breakthrough in cancer treatment, and it has achieved unprecedented success in hematological malignancies, especially in ...relapsed/refractory (R/R) B cell malignancies. At present, CD19 and BCMA are the most common targets in CAR-T cell therapy, and numerous novel therapeutic targets are being explored. However, the adverse events related to CAR-T cell therapy might be serious or even life-threatening, such as cytokine release syndrome (CRS), CAR-T-cell-related encephalopathy syndrome (CRES), infections, cytopenia, and CRS-related coagulopathy. In addition, due to antigen escape, the limited CAR-T cell persistence, and immunosuppressive tumor microenvironment, a considerable proportion of patients relapse after CAR-T cell therapy. Thus, in this review, we focus on the progress and challenges of CAR-T cell therapy in hematological malignancies, such as attractive therapeutic targets, CAR-T related toxicities, and resistance to CAR-T cell therapy, and provide some practical recommendations.
Flexible and stretchable organic solar cells (OSCs) have attracted enormous attention due to their potential applications in wearable and portable devices. To achieve flexibility and stretchability, ...many efforts have been made with regard to mechanically robust electrodes, interface layers, and photoactive semiconductors. This has greatly improved the performance of the devices. State‐of‐the‐art flexible and stretchable OSCs have achieved a power conversion efficiency of 15.21% (16.55% for tandem flexible devices) and 13%, respectively. Here, the recent progress of flexible and stretchable OSCs in terms of their components and processing methods are summarized and discussed. The future challenges and perspectives for flexible and stretchable OSCs are also presented.
The recent progress in flexible and stretchable organic solar cells (OSCs) is discussed. For flexible OSCs, the features of the commonly used flexible transparent electrodes and the relevant performance are selectively summarized and discussed. For stretchable OSCs, both the nonintrinsic and intrinsic processing methods are presented and discussed.
Finding effective molecular design strategies to enable efficient charge generation and small energy loss is among the long-standing challenges in developing high performance non-fullerene organic ...solar cells (OSCs). Recently, we reported Y-series non-fullerene acceptors with an electron-deficient-core-based fused structure (typically Y6), opening a new door to achieve high external quantum efficiency (∼80%) while maintaining low energy loss (∼0.57 eV). On this basis, further reducing the energy losses and ultimately improving the performance of OSCs has become a research hotspot. In this paper, we design and synthesize a new member of the Y-series acceptor family, Y18, which adopts a fused benzotriazole segment with unique luminescence properties as its electron-deficient core. Compared to Y6, the benzotriazole-based acceptor Y18 exhibits extended optical absorption and higher voltage. Consequently, the device delivers a promising power conversion efficiency of 16.52% with a very low energy loss of 0.53 eV. Further device optimization by exploiting a ternary blend strategy allowed us to achieve a high efficiency of 17.11% (certified as 16.76% by NREL). Y18 may become one of the most important candidate materials for its broader absorption spectra and higher voltage of Y18 (compared to Y6) in the OSCs field.
A new small molecule acceptor, Y18, was designed and synthesized. Over 17% efficiency was obtained with single junction solar cells based on Y18.
Cocatalysts have been extensively used to promote water oxidation efficiency in solar‐to‐chemical energy conversion, but the influence of interface compatibility between semiconductor and cocatalyst ...has been rarely addressed. Here we demonstrate a feasible strategy of interface wettability modification to enhance water oxidation efficiency of the state‐of‐the‐art CoOx/Ta3N5 system. When the hydrophobic feature of a Ta3N5 semiconductor was modulated to a hydrophilic one by in situ or ex situ surface coating with a magnesia nanolayer (2–5 nm), the interfacial contact between the hydrophilic CoOx cocatalyst and the modified hydrophilic Ta3N5 semiconductor was greatly improved. Consequently, the visible‐light‐driven photocatalytic oxygen evolution rate of the resulting CoOx/MgO(in)–Ta3N5 photocatalyst is ca. 23 times that of the pristine Ta3N5 sample, with a new record (11.3 %) of apparent quantum efficiency (AQE) under 500–600 nm illumination.
Hydrophilic interface modification of a CoOx‐modified Ta3N5 photocatalyst with a magnesia nanolayer significantly improves its water oxidation efficiency under visible light irradiation. The essential roles of the interface modification are proposed to enhance the interfacial coverage of the CoOx/Ta3N5 photocatalyst and to decrease the defect density of Ta3N5 semiconductor. AQE=apparent quantum efficiency.
The impacts of exogenous or endogenous quorum sensing (QS) signaling molecules on mixed-culture electroactive biofilms (EABs), especially extracellular polymeric substances (EPS) and exoelectrogens ...using direct electron transfer mechanism inside EABs are poorly understood. This research focuses on the influence of acylhomoserine lactones (AHLs), the most common QS signaling molecules for gram negative bacteria, on mixed-culture EABs. Results indicated that both exogenous and endogenous AHLs played the role as regulators to improve the electrochemical activities of EABs. The energy recovery of MFCs increased from 20.5% ± 3.9% to 28.3% ± 4.1% with endogenous AHLs and further rose to 36.2% ± 5.1% with exogenous AHLs, and the start-up period of MFCs shortened from 13 days to 10 days with endogenous AHLs and further reduced to 4 days in the presence of exogenous AHLs. The influences of exogenous and endogenous AHLs were non-instantaneous. They improved some intrinsic properties, i.e. the electrode-associated biomass, the biofilm compactness and the ratio of live/dead cells to obtain superior EABs. Meanwhile, both endogenous and exogenous AHLs increased the concentration and redox activities of EPS. Besides, endogenous AHLs enhanced the diversity of EPS components. Noteworthily, the relative abundance of Geoboacter sp. which is the typical microbe using direct electron transfer mechanism is raised by exogenous AHLs, though so far neither known chemical QS-related gene nor protein has been reported in this genus. These findings will increase the current understanding of QS in EABs and open up an opportunity for regulating mixed-culture MFCs via QS.
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•N-acylhomoserine lactones (AHLs) promote energy recovery of mixed-culture MFC.•Both exogenous and endogenous AHLs improve electrochemical activity of biofilms.•Endogenous AHLs enhanced the diversity of extracellular polymeric substances (EPS).•AHLs result in higher concentration and redox activities of EPS.•AHLs raise proportions of live cells and Geobacter sp. to obtain superior biofilms.