In the hydrothermal synthesis of highly ordered mesoporous silica material SBA-15, strong acid is typically required to catalyze the hydrolysis and condensation of silica species. Meanwhile, under strongly acidic conditions, the transition metal ions, e.g., iron ions, are difficult to incorporate into SBA-15 because of the facile dissociation of Fe-O-Si bonds. Here, we demonstrate an acid-free green synthetic strategy for the synthesis of highly ordered mesoporous SBA-15 and Fe-SBA-15 with the assistance of hydroxyl free radicals that are generated by physical or chemical methods. The prepared materials exhibit a large specific surface area compared to the counterparts prepared by conventional method under acidic conditions. Moreover, Fe-SBA-15 shows high metal loading efficiency as over 50%. Density functional theory calculations suggest that the hydroxyl free radicals exhibit higher catalytic activity than H ions for the hydrolysis of tetraethyl orthosilicate. This radical-facilitated synthesis approach overcomes the challenge to the direct synthesis of highly ordered SBA-15 and Fe-SBA-15 without adding any acid, providing a facile and environmentally friendly route for future large-scale production of ordered mesoporous materials.
catalyst surface to form the final product, which seriously hinders the progress of the reaction. [3,4] Although researchers have made significant progress in the design of catalysts, a large cell voltage is still needed to drive this process. Therefore, it is still highly desirable to design high-efficiency water-splitting electrocatalysts. Recently, ruthenium (Ru) has attracted special attention for water-splitting catalysis since its inherently excellent activity and far lower price than platinum (Pt) and iridium (Ir). [5-9] To date, various strategies have been applied to enhance the activity of the Ru-based catalysts, including turning the crystal phase, doping electrocatalysts with hetero atoms, alloying Ru with the transition metals, and so on forth. [7,10,11] In principle, since the electrocatalysis is usually carried out on the surface of a catalyst, controlling the surface structure of the catalyst is a more straightforward way to improve the catalytic performance. The high-index crystal facets have more coordination unsaturated atoms and more active sites, which is believed to be more active. [12-14] Nevertheless, there were fewer reports on controlling the Ru-based catalysts with high-index facets. To this end, the fine control of Ru-based catalysts is of great significance in both practical application and fundamental research. Shape control has realized huge success for developing efficient Pd/Ptbased nanocatalysts, but the control of Ru-based nanocrystals remains a formidable challenge due to the inherent anisotropy in hexagonal closedpacked nanocrystals. Herein, a class of unique RuCo nanoscrews (NSs) for water electrosplitting is successfully synthesized with rough surfaces and the exposure of steps and edges. Those high-index faceted RuCo NSs show superior performance for overall water electrosplitting, where a low cell voltage of 1.524 V (@ 10 mA cm −2) and excellent stability for more than 20 h (@ 10 mA cm −2) for overall water electrosplitting in 1 m KOH is achieved. The enhanced performance of RuCo NSs is due to the optimization of the binding energy with the intermediate species and the reduced energy barrier of water dissociation. Density functional theory calculations reveal that the RuCo NS structure intrinsically endows various ridges and edges, which create low coordinated Ru-and Co-sites. These active Ru-and Co-sites present high efficiencies in electronic exchange and transfer between adsorbing O species and nearby lattice sites, guaranteeing the high H 2 Osplitting activities. This present work opens up a new strategy for creating high-performance electrocatalysts for water splitting.
Our clinical classification system and therapeutic strategy provide an effective and safe way to treat CSP patients resulting in reduced intraoperative bleeding, operative time, hospital days, and hospital cost.
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Background: Bilateral renal agenesis (BRA) is a lethal congenital anomaly caused by the failure of normal development of both kidneys early in embryonic development. Oligohydramnios upon fetal ultrasonography reveals BRA. Although exact causes are not clear, BRA is associated with mutations in many renal development genes. However, molecular diagnostics cannot pick up many clinical cases. Nephronectin (NPNT) may be a candidate protein for widening diagnosis. It is essential in kidney development and knockout of Npnt in mice frequently leads to kidney agenesis or hypoplasia.
Methods: A consanguineous Han family experienced three cases of induced abortion in the second trimester of pregnancy due to suspicion of BRA. Whole-exome sequencing-(WES)-:based homozygosity mapping detected underlying genetic factors, and a knock-in mouse model confirmed the renal agenesis phenotype.
Results: WES and evaluation of homozygous regions in II-3 and II-4 revealed a pathological homozygous frameshift variant in NPNT (NM_001184690:exon8:c.777dup/p.Lys260*), which leads to a premature stop in the next codon. The truncated NPNT protein exhibited decreased expression, as confirmed in vivo by the overexpression of WT and mutated NPNT. A knock-in mouse model homozygous for the detected Npnt mutation replicated the BRA phenotype.
Conclusions: A biallelic loss-of-function NPNT mutation causing an autosomal recessive form of BRA in humans was confirmed by the corresponding phenotype of knock-in mice. Our results identify a novel genetic cause of BRA, revealing a new target for genetic diagnosis, prenatal diagnosis, and preimplantation diagnosis for families with BRA.
Developing high‐performance catalysts for fuel cell catalysis is the most critical and challenging step for the commercialization of fuel cell technology. Here 1D trimetallic platinum–iron–cobalt nanosaws (Pt3FeCo NSs) with low‐coordination features are designed as efficient bifunctional electrocatalysts for practical fuel cell catalysis. The oxygen reduction reaction (ORR) activity of Pt3FeCo NSs (10.62 mA cm−2 and 4.66 A mg−1Pt at 0.90 V) is more than 25‐folds higher than that of the commercial Pt/C, even after 30 000 voltage cycles. Density functional theory calculations reveal that the strong inter‐d‐orbital electron transfer minimizes the ORR barrier with higher selectivity at robust valence states. The volcano correlation between the intrinsic structure featured with low‐coordination Pt‐sites and corresponding electronic activities is discovered, which guarantees high ORR activities. The Pt3FeCo NSs located in the membrane electrode assembly (MEA) also achieve very high peak power density (1800.6 mW cm−2) and competitive specific/mass activities (1.79 mA cm−2 and 0.79 A mg−1Pt at 0.90 ViR‐free cell voltage) as well as a long‐term lifetime in specific H2O2 medium for proton‐exchange‐membrane fuel cells, ranking top electrocatalysts reported to date for MEA. This work represents a class of multimetallic Pt‐based nanocatalysts for practical fuel cells and beyond.
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