Electrochemical reduction of carbon dioxide (CO2) toward chemical and fuel production is a compelling component of the new energy system. Two‐dimensional bismuth with a particular surface has been ...identified as a highly efficient electrocatalyst for converting CO2 to formate. However, the development of a controllable synthetic strategy for possible large‐scale production of such Bi materials remains highly challenging. Herein, a scalable chemical interface confinement reduction method is proposed for topotactic transformation of BiOBr (001) nanosheets to metallic Bi (001) porous nanosheets (PNS). As expected, the Bi (001) PNS exhibits excellent electrochemical performance on CO2 reduction to formate, with Faradaic efficiency of 95.2% and formate partial current density of 72 mA cm−2. Density functional theory calculations suggest that Bi PNS selectively exposes (001) surfaces with small‐angle grain boundaries can significantly lower the free energy barrier for the formation of *OCHO, which are responsible for the high activity and selectivity toward CO2‐to‐formate conversion.
The chemical interface confinement reduction method is proposed to produce the model catalysts of Bi (001) nanosheets via topotactic transformation of BiOBr (001) nanosheets for CO2 electroreduction at a scalable large‐scale. The formate Faradaic efficiency of 95.2% is achieved on Bi (001) nanosheets due to the small‐angle grain boundaries that can significantly lower the free energy barrier for the formation of *OCHO.
Molybdenum disulfide, as an electronic highly-adjustable catalysts material, tuning its electronic structure is crucial to enhance its intrinsic hydrogen evolution reaction (HER) activity. ...Nevertheless, there are yet huge challenges to the understanding and regulation of the surface electronic structure of molybdenum disulfide-based catalysts. Here we address these challenges by tuning its electronic structure of phase modulation synergistic with interfacial chemistry and defects from phosphorus or sulfur implantation, and we then successfully design and synthesize electrocatalysts with the multi-heterojunction interfaces (e.g., 1T
-MoS
@Ni
P), demonstrating superior HER activities and good stabilities with a small overpotentials of 38.9 and 95 mV at 10 mA/cm
, a low Tafel slopes of 41 and 42 mV/dec in acidic as well as alkaline surroundings, outperforming commercial Pt/C catalyst and other reported Mo-based catalysts. Theoretical calculation verified that the incorporation of metallic-phase and intrinsic HER-active Ni-based materials into molybdenum disulfide could effectively regulate its electronic structure for making the bandgap narrower. Additionally, X-ray absorption spectroscopy indicate that reduced nickel possesses empty orbitals, which is helpful for additional H binding ability. All these factors can decrease Mo-H bond strength, greatly improving the HER catalytic activity of these materials.
Steroid (glucocorticoid)-induced osteonecrosis of the femoral head (SONFH) is a metabolic disease that occurs due to the use of glucocorticoid drugs, leading to impaired blood supply to the femoral ...head and death of bone cells and bone marrow composition, which in turn lead to structural change, collapse of the femoral head, and articular dysfunction. SONFH is a challenging disorder to treat in adults due to frequent collapse of the femoral head and dysfunction of the hip joint. Eventually, patients require joint arthroplasty surgery, which severely impairs the patients' quality of life. However, the exactly pathogenesis of SONFH is still not clear. Recently, as the development of precision medicine and lucubrating on stem cell and molecular biology, the exact pathogenesis of SONFH is being investigated and more new treatments are being explored. This review article discusses five major theories about the pathogenesis of SONFH.
•This review article discusses five major theories about the pathogenesis of SONFH.•This review article discusses the regulating effect of non-coding RNAs in the pathogenetic process of SONFH.•The pathogenesis of SONFH is the outcome of the combined action of multiple mechanisms.
Psoriasis is a chronic skin inflammatory disorder, the immune mechanism of which has been profoundly elucidated in the past few years. The dominance of the interleukin (IL)‐23/IL‐17 axis is a ...significant breakthrough in the understanding of the pathogenesis of psoriasis, and treatment targeting IL‐23 and IL‐17 has successfully benefited patients with the disease. The skin contains a complex network of dendritic cells (DC) mainly composed of epidermal Langerhans cells, bone marrow‐derived dermal conventional DC, plasmacytoid DC and inflammatory DC. As the prominent cellular source of α‐interferon, tumor necrosis factor‐α, IL‐12 and IL‐23, DC play a pivotal role in psoriasis. Thus, targeting pathogenic DC subsets is a valid strategy for alleviating and preventing psoriasis and other DC‐derived diseases. In this review, we survey the known role of DC in this disease.
Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic ...efficiencies. Here, copper single atoms anchored to Ti
C
T
MXene nanosheets are firstly demonstrated as effective and robust catalysts for electrochemical carbon monoxide reduction, achieving an ultrahigh selectivity of 98% for the formation of multicarbon products. Particularly, it exhibits a high Faradaic efficiency of 71% towards ethylene at -0.7 V versus the reversible hydrogen electrode, superior to the previously reported copper-based catalysts. Besides, it shows a stable activity during the 68-h electrolysis. Theoretical simulations reveal that atomically dispersed Cu-O
sites favor the C-C coupling of carbon monoxide molecules to generate the key *CO-CHO species, and then induce the decreased free energy barrier of the potential-determining step, thus accounting for the high activity and selectivity of copper single atoms for carbon monoxide reduction.
Improved chloride binding stability for calcium aluminate cements is proposed by the doping of phosphorus. Phosphorus‐modified aluminates clinker has an improved chloride binding stability compared ...to pristine aluminates, ordinary Portland cement and sulfur‐modified calcium aluminates, as verified by experimental observation. The existence of the newly found phosphorus‐modified Friedel's salt (PFS) accounts for the excellent chloride binding stability, which was understood by density functional theory calculations. Local density of states of the valence band minimum is predominantly localized around P atoms in the PFS, but evenly distributed in the Friedel's salt (FS). The frontier band energy of the partial density of states on Cl and O elements in the PFS is lower than that in the FS by 0.21 and 0.05 eV, respectively. This makes the PFS more stable than the FS salt to ionic attack.
Newly discovered P‐doped Friedel's salt modification structure. P‐modified Friedel's salt significantly improves the chloride binding stability as an aspect of electronic structure manipulation by incorporating alien element.
Na superionic conductor structured Na3V2(PO4)3 cathodes have attracted great interest due to their long cycling lifespan and high thermal stability rendered by the robust 3D framework. However, their ...practical application is still hindered by the high cost of raw materials and limited energy density. Herein, a doping strategy with low‐cost Fe2+ is developed to activate V4+/V5+ redox, in an attempt to increase the energy density of phosphate cathodes. It is also revealed that reversible activation of V4+/V5+ redox is related to the Na positions (Na1, 6b; Na2, 18e). Only the V‐based compounds with enough Na2 content can activate the V4+/V5+ reversibly. More importantly, without presodiation treatment and addition of any sodiation agent, Na3.4V1.6Fe0.4(PO4)3 is delicately designed as both cathode and the Na self‐compensation agent in full cells, allowing a promising energy density of ≈260 Wh kg−1. This work sheds light on enhancing the energy density, and designing Na self‐compensation for practical Na‐ions batteries.
Na3.4V1.6Fe0.4(PO4)3 is delicately designed as both cathode and the Na self‐compensation agent in full cells, which can supplement the Na+ consumption during the formation of the solid electrolyte interphase layer on the hard carbon by sacrificing the capacity from the low‐voltage Fe2+/Fe3+ and achieve a promising energy density of 260 Wh kg−1 contributed to by the reversible V3+/V4+/V5+ redox couples.
It is an important task for China to allocate carbon emission allowance to realize its carbon reduction target and establish carbon trading market. China has designed several allocation rules within ...seven pilot regions. What influence those rules may cause is closely related with the enthusiasm of emission trading scheme (ETS) covered enterprises' participation in carbon market, and more importantly, with the mechanism design and sustainable development of carbon market. For this purpose, the multi-stage profit model is developed to analyze the ETS-covered enterprises' product prices and emission reduction behaviors under different allocation rules. The results show that, first, under the rules of grandfathering, self-declaration and auctioning, when deciding the optimal product price and optimal carbon emission reduction, those enterprises may focus on maximizing current stage profit; however, under the rule of benchmarking, those enterprises may care more about the impact of current decisions on the profit in next stage. Second, the optimal product price policy is positively correlated with the price of the same kind products, consumers' low-carbon awareness and government subsidy. Finally, along with the increase of carbon price, consumers' low-carbon awareness and government subsidy and the decrease of carbon emission cap, those enterprises tend to reduce carbon emissions.
•Analyze the impact of carbon allowance allocation rules on ETS-covered enterprises.•For grandfather, self-declaration and auction, they may maximize current profits.•For benchmark, they care the effect of current decisions on the coming profits.•The optimal product price positively relates to low-carbon awareness and subsidy.•Carbon price, low-carbon awareness and subsidy rise leads their emission reduction.
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•Higher As groundwater was found near the permanent wetland (PW) than dried wetland (DW).•PW sediments had more autochthonous or aquatic biological organic matter than DW ...sediments.•DOM in PW groundwater was more bioreactive than that in DW groundwater.•Higher dissolved As concentrations were related to higher bioreactivity of organic matter.•Bioreactive organic matter triggered As mobilization via reductive dissolution of Fe oxides.
Organic matter (OM) is widely accepted to be the trigger for arsenic (As) mobilization from sediments into groundwater. Identifications of reactivity and sources of organic matter responsible for driving As liberation remain unresolved. To address these issues, we provide the extensive characterization of OM in shallow groundwater, surface water, and sediments near a permanent wetland and a dried wetland in the Hetao basin with high As groundwater and low As groundwater, respectively, using fluorescence spectroscopy and parallel factor analysis (PARAFAC). Dissolved organic matter (DOM) of shallow groundwater and sediments near the permanent wetland had higher biological index (BIX), and more protein-like components and microbially-derived components relative to that near the dried wetland, showing higher bioreactivity. Fingerprint of water stable isotopes and higher water levels of wetland than shallow groundwater pointed to the recharge of wetland water into shallow groundwater. Laboratory incubations of the sediment with more bioreactive OM obtained near the permanent wetland mobilized more As. Both DOM properties and laboratory incubations indicate that OM with high bioreactivity promoted As mobility mainly by fuelling microbial respiration of Fe oxide reduction. Recharge of wetland water into shallow groundwater introduced bioreactive DOM into shallow aquifer. Groundwater DOM near the permanent wetland was typically sourced from both wetland DOM and sedimentary OM with high bioreactivity. However, sedimentary OM was the major source of groundwater DOM near the dried-wetland. It suggested that downward infiltration of surface-derived OM and perturbations of aquifer sediments by changing groundwater flow regimes increase bioreactivity of groundwater DOM and therefore enhance As mobility.
Kesterite Cu2ZnSn(S,Se)4 (CZTSSe) with earth‐abundant and environmental‐benign constituents has been regarded as a promising solar energy harvesting material for green and cost‐effective photovoltaic ...applications. The record efficiency of CZTSSe solar cells has recently been refreshed twice after years‐long stagnation, keeping it in the spotlight. Nevertheless, the champion efficiency of 13.6% is still far behind its counterpart Cu(In,Ga)Se2 (CIGS) (23.35%) despite being endowed with a similar electronic structure and nearly‐identical device architecture. In fact, CZTSSe solar cells are more susceptible to non‐radiative recombination at bulk and interfaces, which must be improved for further efficiency advancement. In this review, the state‐of‐art strategies to enhance the power conversion efficiency of CZTSSe solar cells are summarized and discussed, with focus given to three critical device regions i) kesterite absorber, ii) buffer/kesterite interface, and iii) kesterite/back contact interface. With the further elucidation of the latest progress and disclosure of fundamental mechanisms, novel insights toward high‐efficiency kesterite solar cells are proposed.
State‐of‐art strategies addressing the dominant recombination in kesterite Cu2ZnSn(S,Se)4 solar cells are reviewed. Attention is focused on the kesterite absorber, front p‐n heterojunction, and kesterite/back contact interface, as they primarily limit the performance of kesterite devices and can be improved simultaneously. By systematically scrutinizing these highly compatible measures, promising research directions are proposed to stimulate further progress and strategy integration.
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