Water electrolysis is a promising source of hydrogen; however, technological challenges remain. Intensive efforts have focused on developing highly efficient and earth‐abundant electrocatalysts for ...water splitting. An effective strategy is proposed, using a bifunctional tubular cobalt perselenide nanosheet electrode, in which the sluggish oxygen evolution reaction is substituted with anodic hydrazine oxidation so as to assist energy‐efficient hydrogen production. Specifically, this electrode produces a current density of 10 mA cm−2 at −84 mV for hydrogen evolution and −17 mV for hydrazine oxidation in 1.0 m KOH and 0.5 m hydrazine electrolyte. An ultralow cell voltage of only 164 mV is required to generate a current density of 10 mA cm−2 for 14 hours of stable water electrolysis.
Sweet electrocatalytic synergy: An effective strategy for energy‐saving water electrolysis is presented. The sluggish oxygen evolution reaction is replaced by anodic hydrazine oxidation on a low‐cost and bifunctional cobalt perselenide electrode.
Hydrogen economy by water splitting is the indispensable cornerstone for sustainable energy yet it is impeded by sluggish anodic water oxidation. Hence, the rational design of highly efficient ...electrocatalysts for oxygen evolution is the key to unlocking its wider use. Herein, cobalt-iron selenide nanoframes are reported for the efficient water oxidation, which need only 270 mV overpotential to give a 10 mA cm
−2
current density and outperforms most cobalt-based catalysts, and even the benchmarked commercial ruthenium oxides (RuO
2
). More profoundly, iron doping regulates the local spin state of cobalt species, which further accelerates charge transfer and formation of oxygenated intermediates, and consequently contributes to the enhanced oxygen evolution. This work demonstrates a highly efficient oxygen evolution electrocatalyst and may pioneer a promising approach which involves tuning the local electronic structure to achieve the improved electrocatalysis activities in energy conversion technologies.
Tuning local spin state of Co centres by Fe doping in cobalt-iron selenides is effective for boosting oxygen evolution.
The electrocatalytic carbon dioxide reduction reaction (CO2RR) to value‐added chemical products is an effective strategy for both greenhouse effect mitigation and high‐density energy storage. ...However, controllable manipulation of the oxidation state and porous structure of Cu‐carbon based catalysts to achieve high selectivity and current density for a particular product remains very challenging. Herein, a strategy derived from Cu‐based metal‐organic frameworks (MOFs) for the synthesis of controllable oxidation states and porous structure of Cu‐carbon (Cu‐pC, Cu2O‐pC, and Cu2O/Cu‐pC) is demonstrated. By regulating oxygen partial pressure during the annealing process, the valence state of the Cu and mesoporous structures of surrounding carbon are changed, leads to the different selectivity of products. Cu2O/CuO‐pC with the higher oxidation state exhibits FEC2H4 of 65.12% and a partial current density of −578 mA cm−2, while the Cu2O‐pC shows the FECH4 over 55% and a partial current density exceeding −438 mA cm−2. Experimental and theoretical studies indicate that porous carbon‐coated Cu2O structures favor the CH4 pathway and inhibit the hydrogen evolution reaction. This work provides an effective strategy for exploring the influence of the various valence states of Cu and mesoporous carbon structures on the selectivity of CH4 and C2H4 products in CO2RR.
A controllable oxidation strategy derived from Cu‐based metal organic frameworks (MOFs) is introduced for the synthesis of controllable oxidation states and porous structure of Cu‐carbon (Cu‐pC, Cu2O‐pC, and Cu2O/Cu‐pC) for selective CO2 electroreduction. The Cu2O/CuO‐pC with the higher oxidation state exhibits FEC2H4 of 65.12% and the Cu2O‐pC shows the FECH4 over 55%.
Despite incorporation of organic groups into silica‐based aerogels to enhance their mechanical flexibility, the wide temperature reliability of the modified silicone aerogel is inevitably degraded. ...Therefore, facile synthesis of soft silicone aerogels with wide‐temperature stability remains challenging. Herein, novel silicone aerogels containing a high content of Si are reported by using polydimethylvinylsiloxane (PDMVS), a hydrosilylation adduct with water‐repellent groups, as a “flexible chain segment” embedded within the aerogel network. The poly(2‐dimethoxymethylsilyl)ethylmethylvinylsiloxane (PDEMSEMVS) aerogel is fabricated through a cost‐effective ambient temperature/pressure drying process. The optimized aerogel exhibits exceptional performance, such as ultra‐low density (50 mg cm−3), wide‐temperature mechanical flexibility, and super‐hydrophobicity, in comparison to the previous polysiloxane aerogels. A significant reduction in the density of these aerogels is achieved while maintaining a high crosslinking density by synthesizing gel networks with well‐defined macromolecules through hydrolytic polycondensation crosslinking of PDEMSEMVS. Notably, the pore/nanoparticle size of aerogels can be fine‐tuned by optimizing the gel solvent type. The as‐prepared silicone aerogels demonstrate selective absorption, efficient oil–water separation, and excellent thermal insulation properties, showing promising applications in oil/water separation and thermal protection.
A soft polysiloxane aerogel is designed and successfully fabricated through the condensation process of polydimethylvinylsiloxane macromolecules. In addition to its ultra‐lightweight nature, this material possesses several advantageous properties, including exceptional mechanical stability when exposed to liquid nitrogen, effective thermal insulation, super‐hydrophobicity, and notable advancements in porous material development.
Hydrogen production via water electrolysis is promising but impeded by sluggish cathodic and anodic reactions. Consequently, highly-efficient and earth-abundant electrocatalysts are attracting ...considerable attention. Herein we report a bifunctional NiMo alloy nanotube for efficient hydrogen production coupled with anodic urea oxidation in a hybrid water electrolysis system. Specifically, ultralow potentials of −44 mV and 1.36 V (vs. RHE) are required to deliver 10 mA cm−2 current density for cathodic and anodic reactions, respectively. Density functional theory (DFT) calculation results show the Mo center is the main reaction site for the chemisorption and OH bond cleavage of H2O while Ni center is identified as the hydrogen-evolving site. Based on this bifunctional NiMo electrocatalyst, a hybrid water electrolysis cell is proposed and the overall cell voltage of ∼1.43 V is achieved for outputting 10 mA cm−2 current density during the 10 h operation. The understandings in alternative electrode reactions coupled with highly-efficient and earth-abundant electrocatalysts for hybrid water electrolysis in this work holds encouraging potential in future energy conversion technologies and urea-related water treatments.
Nickel-molybdenum nanotube demonstrates the bifunctional and excellent electrocatalytic activity in the hybrid water electrolysis for energy-efficient and cost-effective hydrogen production assisting by anodic urea oxidation. Display omitted
•we report a bifunctional NiMo alloy nanotube for efficient hydrogen production coupled with anodic urea oxidation.•The Mo center is main reaction site for chemisorption and OH bond cleavage of H2O, while the Ni center is identified as the hydrogen-evolving site.•A hybrid water electrolysis cell with a voltage of 1.43 V is achieved for steadily outputting 10 mA cm−2 current density of hydrogen production.
Some molecular and functional properties of albumin (83.6% protein), globulin (95.5% protein), glutelin (81.3% protein) as well as protein isolate (80.7% protein) from cashew nut were investigated. ...These proteins were subjected to molecular (circular dichroism, gel electrophoresis, scanning electron microscopy) and functional (solubility, emulsification, foaming, water/oil holding capacity) tests. Cashew nut proteins represent an abundant nutrient with well-balanced amino acid composition and could meet the requirements recommended by FAO/WHO. SDS-PAGE pattern indicated cashew nut proteins were mainly composed of a polypeptide with molecular weight (MW) of 53 kDa, which presented two bands with MW of 32 and 21 kDa under reducing conditions. The far-UV CD spectra indicated that cashew proteins were rich in β-sheets. The surface hydrophobicity of the protein isolate was higher than that of the protein fractions. In pH 7.0, the solubility of protein fractions was above 70%, which was higher than protein isolate at any pH. Glutelin had the highest water/oil holding capacity and foaming properties. Protein isolate displayed better emulsifying properties than protein fractions. In summary, cashew nut kernel proteins have potential as valuable nutrition sources and could be used effectively in the food industry.
Hard carbons (HCs) with high sloping capacity are considered as the leading candidate anode for sodium‐ion batteries (SIBs); nevertheless, achieving basically complete slope‐dominated behavior with ...high rate capability is still a big challenge. Herein, the synthesis of mesoporous carbon nanospheres with highly disordered graphitic domains and MoC nanodots modification via a surface stretching strategy is reported. The MoOx surface coordination layer inhibits the graphitization process at high temperature, thus creating short and wide graphite domains. Meanwhile, the in situ formed MoC nanodots can greatly promote the conductivity of highly disordered carbon. Consequently, MoC@MCNs exhibit an outstanding rate capacity (125 mAh g−1 at 50 A g−1). The “adsorption‐filling” mechanism combined with excellent kinetics is also studied based on the short‐range graphitic domains to reveal the enhanced slope‐dominated capacity. The insight in this work encourages the design of HC anodes with dominated slope capacity toward high‐performance SIBs.
Mesoporous carbon nanospheres with highly disordered graphitic domains and MoC nanodots modification are developed via a surface stretching strategy. The MoOx surface coordination layer inhibits the graphitization process at high temperature, while the in situ formed MoC nanodots can greatly promote the conductivity of highly disordered carbon. Consequently, MoC@MCNs exhibit enhanced slope‐dominated capacity, as well as outstanding rate capability and cycle performance.
Summary
Patients who receive allogeneic haematopoietic stem cell transplantation (allo‐HSCT) may develop sepsis, which result in a highly intensive care unit admission rate and mortality. Therefore, ...short‐term and long‐term prognostic models for sepsis after allo‐HSCT are urgently needed. We enrolled patients receiving allo‐HSCT who developed sepsis after allo‐HSCT at Peking University People's Hospital between 2012 and 2021, including 287 patients who received allo‐HSCT in 2018–2021 in the derivation cohort, and 337 patients in 2012–2017 in the validation cohort. Multivariate logistic regression analysis was used to identify prognostic factors, and these identified factors were incorporated into two scoring models. Seven independent factors (acute graft‐versus‐host disease (GVHD), chronic GVHD (cGVHD), total bilirubin, lactate dehydrogenase (LDH) and organ dysfunction renal, lung and heart) were included in the 6‐month prognostic model, and six factors (cGVHD, C‐reactive protein, LDH, organ dysfunction lung, neurologic and coagulation) were included in the 14‐day prognostic model. The area under the receiver operating characteristic curves, calibration plots and decision curve analysis demonstrated the robust predictive performance of the models, better than the Sequential Organ Failure Assessment score. Early identification of patients with high risk of 6‐month and 14‐day death may allow clinicians to provide timely treatments and improve the therapeutic effects.
A prognostic system, including a 6‐month prognostic model and a 14‐day prognostic model, was developed to help recognize sepsis with allo‐HSCT with a high risk of poor outcome. The two prognostic models were demonstrated to have good predictive performance and help identify patients with high risk.
Ultracold polar molecules possess long-range, anisotropic and tunable dipolar interactions, providing opportunities to probe quantum phenomena that are inaccessible with existing cold gas platforms. ...However, experimental progress has been hindered by the dominance of two-body loss over elastic interactions, which prevents efficient evaporative cooling. Although recent work has demonstrated controlled interactions by confining molecules to a two-dimensional geometry, a general approach for tuning molecular interactions in a three-dimensional stable system has been lacking. Here we demonstrate tunable elastic dipolar interactions in a bulk gas of ultracold 40K87Rb molecules in three dimensions, facilitated by an electric field-induced shielding resonance that suppresses the reactive loss by a factor of 30. This improvement in the ratio of elastic to inelastic collisions enables direct thermalization. The thermalization rate depends on the angle between the collisional axis and the dipole orientation controlled by an external electric field, a direct manifestation of the anisotropic dipolar interaction. We achieve evaporative cooling mediated by the dipolar interactions in three dimensions. This work demonstrates full control of a long-lived bulk quantum gas system with tunable long-range interactions, paving the way for the study of collective quantum many-body physics.Realizing the potential of dipolar molecular gases to explore quantum physics needs elastic, tunable interactions and low temperatures. This is now possible due to advances in control that suppress molecular losses and enable efficient cooling.
Development of cancer has been linked to chronic inflammation, particularly via interleukin-23 (IL-23) and IL-17 signaling pathways. However, the cellular source of IL-17 and underlying mechanisms by ...which IL-17-producing cells promote human colorectal cancer (CRC) remain poorly defined. Here, we demonstrate that innate γδT (γδT17) cells are the major cellular source of IL-17 in human CRC. Microbial products elicited by tumorous epithelial barrier disruption correlated with inflammatory dendritic cell (inf-DC) accumulation and γδT17 polarization in human tumors. Activated inf-DCs induced γδT17 cells to secrete IL-8, tumor necrosis factor alpha, and GM-CSF with a concomitant accumulation of immunosuppressive PMN-MDSCs in the tumor. Importantly, γδT17 cell infiltration positively correlated with tumor stages and other clinicopathological features. Our study uncovers an inf-DC-γδT17-PMN-MDSC regulatory axis in human CRC that correlates MDSC-meditated immunosuppression with tumor-elicited inflammation. These findings suggest that γδT17 cells might be key players in human CRC progression and have the potential for treatment or prognosis prediction.
•Innate γδT cells are the major cellular source of IL-17 in human CRC•Microbial invasion activates inf-DCs to facilitate γδT17 polarization via IL-23•γδT17 cells mobilize PMN-MDSCs into the tumor to elicit immunosuppression•Tumorous γδT17 cells are correlated with clinicopathological features of human CRC
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