Understanding the site interaction nature of single‐atom catalysts (SACs), especially densely populated SACs, is vital for their application to various catalytic reactions. Herein, we report a site ...distance effect, which emphasizes how well the distance of the adjacent copper atoms (denoted as dCu1−Cu1) matches with the reactant peroxydisulfate (PDS) molecular size to determine the Fenton‐like reaction reactivity on the carbon‐supported SACs. The optimized dCu1−Cu1 in the range of 5–6 Å, which matches the molecular size of PDS, endows the catalyst with a nearly two times higher turnover frequency than that of dCu1−Cu1 beyond this range, accordingly achieving record‐breaking kinetics for the oxidation of emerging organic contaminants. Further studies suggest that this site distance effect originates from the alteration of PDS adsorption to a dual‐site structure on Cu1−Cu1 sites when dCu1−Cu1 falls within 5–6 Å, significantly enhancing the interfacial charge transfer and consequently resulting in the most efficient catalyst for PDS activation so far.
Site distance effects are important in a Cu1/N‐doped graphene (Cu1/GN) single‐atom catalyst with record‐breaking kinetics in the oxidation of emerging organic pollutants. A strategy is reported to achieve the desired catalyst behavior by matching the active site with the properties of the reaction molecule peroxydisulfate (PDS).
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Neuroinflammation is involved in the pathogenesis of amyotrophic lateral sclerosis (ALS), but only limited data are available on systematic peripheral and central immune cell profiles in ALS. We ...studied detailed immune profiles of 73 ALS patients and 48 healthy controls (controls) in peripheral blood by fluorescence-activated cell sorting as well as cytokine expression profiles in serum. In a subgroup of 16 ALS patients and 10 controls we additionally studied cerebrospinal fluid (CSF) samples. In peripheral blood, T cell subtypes presented a shift towards pro-inflammatory Th 1 and Th 17 cells whereas anti-inflammatory Th2 and T regulatory cells were decreased. Important players in innate immunity including distinct monocyte (Mo) and natural killer (NK) cell subtypes were changed in ALS patients compared to controls. Pro-inflammatory serum cytokines such as interleukin (IL)-1 beta, IL-6 and interferon-gamma (IFN-gamma) were increased and the anti-inflammatory cytokine IL-10 was decreased. Correlation analysis revealed moderate negative correlations between Th1 and Th17 to the ALS functional rating scale revised (ALSFRS-R) and to forced vital capacity. In CSF samples, no relevant alteration of the immune profile was found. In conclusion, the immune profile in ALS was shifted towards a Th1/Th17 cell-mediated pro-inflammatory immune response and correlated to disease severity and progression. Large prospective studies are needed to confirm these findings.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Electrochemical nitric oxide reduction reaction (NORR) to produce ammonia (NH
3
) under ambient conditions is a promising alternative to the energy and carbon-intensive Haber-Bosch approach, but its ...performance is still improved. Herein, molybdenum carbides (MoC) nanocrystals confined by nitrogen-doped carbon nanosheets are first designed as an efficient and durable electrocatalyst for catalyzing the reduction of NO to NH
3
with maximal Faradaic efficiency of 89% ± 2% and a yield rate of 1,350 ± 15 µg·h
−1
·cm
−2
at the applied potential of −0.8 V vs. reversible hydrogen electrode (RHE) as well as high stable activity with negligible current density and NH
3
yield rate decays over a 30 h continue the test. Moreover, as a proof-of-concept of Zn−NO battery, it achieves a peak power density of 1.8 mW·cm
−2
and a large NH
3
yield rate of 782 ± 10 µg·h
−1
·cm
−2
, which are comparable to the best-reported results. Theoretical calculations reveal that the MoC(111) has a strong electronic interaction with NO molecules and thus lowering the energy barrier of the potential-determining step and suppressing hydrogen evolution kinetics. This work suggests that Mo-based materials are a powerful platform providing great opportunities to explore highly selective and active catalysts for NH
3
production.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
The electrosynthesis of hydrogen peroxide (H
2
O
2
) from oxygen reduction reaction (ORR) via a two-electron pathway provides an appealing alternative to the energy-intensive anthraquinone route; ...however, the development of ORR with high selectivity and durability for H
2
O
2
production is still challenging. Herein, we demonstrate an active and stable catalyst, composing of highly dispersed Ag nanoclusters on N-doped hollow carbon spheres (NC-Ag/NHCS), which can effectively reduce O
2
molecules into H
2
O
2
with a selectivity of 89%–91% in a potential range from 0.2 to 0.7 V (vs. reversible hydrogen electrode (RHE)) in acidic media. Strikingly, NC-Ag/NHCS achieve a mass activity of 27.1 A·g
−1
and a yield rate of 408 mmol·g
cat.
−1
·h
−1
at 0.7 V, both of which are comparable with the best-reported results. Furthermore, NC-Ag/NHCS enable catalyzing H
2
O
2
production with a stable current density over 48-h electrolysis and only about 9.8% loss in selectivity after 10,000 cycles. Theoretical analyses indicate that Ag nanoclusters can contribute more electrons to favor the protonation of adsorbed O
2
, thus leading to a high H
2
O
2
selectivity. This work confirms the great potential of metal nanocluster-based materials for H
2
O
2
electrosynthesis under ambient conditions.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Electrocatalytic NO reduction reaction to generate NH3 under ambient conditions offers an attractive alternative to the energy-extensive Haber–Bosch route; however, the challenge still lies in the ...development of cost-effective and high-performance electrocatalysts. Herein, nanoporous VN film is first designed as a highly selective and stable electrocatalyst for catalyzing reduction of NO to NH3 with a maximal Faradaic efficiency of 85% and a peak yield rate of 1.05 × 10–7 mol·cm–2·s–1 (corresponding to 5,140.8 μg·h–1·mgcat.–1) at –0.6 V vs. reversible hydrogen electrode in acid medium. Meanwhile, this catalyst maintains an excellent activity with negligible current density and NH3 yield rate decays over 40 h. Moreover, as a proof-of-concept of Zn–NO battery, it delivers a high power density of 2.0 mW·cm–2 and a large NH3 yield rate of 0.22 × 10–7 mol·cm–2·s–1 (corresponding to 1,077.1 μg·h–1·mgcat.–1), both of which are comparable to the best-reported results. Theoretical analyses confirm that the VN surface favors the activation and hydrogenation of NO by suppressing the hydrogen evolution. This work highlights that the electrochemical NO reduction is an eco-friendly and energy-efficient strategy to produce NH3.
Designing efficient and cost-effective bifunctional catalysts is desirable for carbon dioxide and oxygen reduction reactions (CO
2
RR and ORR) to address carbon neutralization and energy conversion. ...Herein, a bifunctional CO
2
RR and ORR catalyst for aqueous Zn-air battery (ZAB) self-driving CO
2
RR electrolysis is developed using atomically dispersed niobium anchored onto N-doped ordered mesoporous carbon (Nb-N-C). The Nb-N-C atomic catalyst demonstrates aqueous CO
2
RR activity with CO Faradaic efficiency up to 90%, ORR activity with a half-wave potential of 0.84 V
vs.
reversible hydrogen electrode, and ZAB activity with a peak power density of 115.6 mW cm
−2
, owing to the high Nb atom-utilization efficiency and ordered mesoporous structure. Furthermore, two-unit ZABs in series, serving as the power source for the self-powered CO
2
electrolysis system, continuously convert CO
2
to CO with average productivity of 3.75 µmol h
−1
m
g
c
a
t
-
1
during the first 10 h. Moreover, theoretical calculations exhibit that atomic Nb anchored to N-doped carbon can form Nb-N coordination bonds, effectively reducing the energy barriers of potential-determining *COOH for CO
2
RR and *O formation for ORR.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
In this roadmap, two-dimensional materials including graphene, black phosporus, MXenes, covalent organic frameworks, oxides, chalcogenides, and others, are highlighted in energy storage and ...conversion.
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Energy storage and conversion have attained significant interest owing to its important applications that reduce CO2 emission through employing green energy. Some promising technologies are included metal-air batteries, metal-sulfur batteries, metal-ion batteries, electrochemical capacitors, etc. Here, metal elements are involved with lithium, sodium, and magnesium. For these devices, electrode materials are of importance to obtain high performance. Two-dimensional (2D) materials are a large kind of layered structured materials with promising future as energy storage materials, which include graphene, black phosporus, MXenes, covalent organic frameworks (COFs), 2D oxides, 2D chalcogenides, and others. Great progress has been achieved to go ahead for 2D materials in energy storage and conversion. More researchers will join in this research field. Under the background, it has motivated us to contribute with a roadmap on ‘two-dimensional materials for energy storage and conversion.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Brevibacterium frigoritolerans
, a strain quite potential use in environmental pollution, is also able to degrade the pesticide phorate. Here, we report a strain isolated from radioactive soil in the ...Xinjiang Uygur Autonomous Region of China. The genome of strain GD44 encompasses 5,471,331 base pairs with a GC content of 40.42%. The sequence was assembled into 1985 open reading frames (ORFs) encoding 5053 proteins. Sequence analysis identified the genes encoding enzymes related to the degradation of organophosphorus compounds such as esterase, phosphotransferase, C–P lyase, and alkaline phosphatase. The nitrate reductase gene was also found in GD44, which was associated with biosynthesis of silver nanoparticles used for bacteriostat. In addition, Antibiotic Resistance Ontology (ARO) genes accounted for 10.6%, including the vancomycin resistance gene cluster. Therefore, the whole-genome sequence of
B. frigoritolerans
GD44 will be beneficial for identifying and analyzing genes utilized for soil remediation and antibacterial agent, which will provide genetic evaluation for potential application in the future.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OBVAL, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Aging, body composition, and body mass index (BMI) are important factors in bone mineral density (BMD). Although several studies have investigated the various parameters and factors that ...differentially influence BMD, the results have been inconsistent. Thus, the primary goal of the present study was to further characterize the relationships of aging, body composition parameters, and BMI with BMD in Chinese Han males older than 50 years.
The present study was a retrospective analysis of the body composition, BMI, and BMD of 358 Chinese male outpatients between 50 and 89 years of age that were recruited from our hospital between 2009 and 2011. Qualified subjects were stratified according to age and BMI as follows: 50-59 (n = 35), 60-69 (n = 123), 70-79 (n = 93), and 80-89 (n = 107) years of age and low weight (BMI: < 20 kg/m2; n = 21), medium weight (20 ≤ BMI < 24 kg/m2; n = 118), overweight (24 ≤ BMI < 28 kg/m2; n = 178), and obese (BMI ≥ 28 kg/m2; n = 41). Dual-energy X-ray absorptiometry (DEXA) was used to assess bone mineral content (BMC), lean mass (LM), fat mass (FM), fat-free mass (FFM), lumbar spine (L1-L4) BMD, femoral neck BMD, and total hip BMD. Additionally, the FM index (FMI; FM/height2), LM index (LMI; LM/height2), FFM index (FFMI; BMC+LM/height2), percentage of BMC (%BMC; BMC/BMC+FM+LM × 100%), percentage of FM (%FM; FM/BMC+FM+LM × 100%), and percentage of LM (%LM; LM/(BMC+FM+LM) × 100%) were calculated. Osteopenia or osteoporosis was identified using the criteria and T-score of the World Health Organization.
Although there were no significant differences in BMI among the age groups, there was a significant decline in height and weight according to age (p < 0.0001 and p = 0.0002, respectively). The LMI and FFMI also declined with age (both p < 0.0001) whereas the FMI exhibited a significant increase that peaked in the 80-89-years group (p = 0.0145). Although the absolute values of BMC and LM declined with age (p = 0.0031 and p < 0.0001, respectively), there was no significant difference in FM. In terms of body composition, there were no significant differences in %BMC but there was an increase in %FM (p < 0.0001) and a decrease in %LM (p < 0.0001) with age. The femoral neck and total hip BMD significantly declined with age (p < 0.0001 and p = 0.0027, respectively) but there were no differences in L1-L4. BMD increased at all sites (all p < 0.01) as BMI increased but there were declines in the detection rates of osteoporosis and osteopenia (both p < 0.001). A logistic regression revealed that when the medium weight group was given a BMI value of 1, a decline in BMI was an independent risk factor of osteoporosis or osteopenia, while an increase in BMI was a protective factor for BMD. At the same time, BMD in L1-L4 exhibited a significant positive association with FMI (p = 0.0003) and the femoral neck and total hip BMDs had significant positive associations with FFMI and LMI, respectively (both p < 0.0001).
These data indicate that LMI and FFMI exhibited significant negative associations with aging in Chinese Han males older than 50 years, whereas FMI had a positive association. BMD in the femoral neck and total hip declined with age but an increased BMI was protective for BMD. LMI and FFMI were protective for BMD in the femoral neck and total hip.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
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In atmospheric conditions, CuI is easily oxidized to CuII due to the coexistence of moisture and oxygen. The poor oxidation inhibition of CuI restricts the practical application of ...CuI-containing materials. Herein we introduce an approach to construct a superhydrophobic microenvironment in CuI-functionalized metal–organic frameworks by coordinatedly grafting organic amine compounds onto open metal sites (OMSs), which can hinder the accessibility of moisture to pores thereby enhancing the stability of CuI. As a proof of concept, MIL-101(Cr) with abundant OMSs and octadecylamine (OA) with long hydrophobic alkyl groups are used as carrier and surface coating. As superhydrophobic porous materials, the resultant CuIM-OA exhibits improved CuI stability in addition to retaining high crystallinity and intact porosity while almost all CuI is oxidized in hydrophilic CuIM upon exposure in a humid atmosphere for 30 h. CuIM-OA owns excellent adsorption desulfurization performance (ADS) with regard to thiophene, benzothiophene, and 4,6-dimethyl dibenzothiophene. Even from hydrated fuel, the adsorption performance of CuIM-OA maintains well while the adsorption capacity of CuIM decreases to 7% after 4 cycles. The remarkable moisture resistance, CuI stability, and high porosity make the current adsorbent CuIM-OA highly promising for the practical ADS process.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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