15 research outputs found

    Optical Trapping of a Single Protein

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    We experimentally demonstrate the optical trapping of a single bovine serum albumin (BSA) molecule that has a hydrodynamic radius of 3.4 nm, using a double-nanohole in an Au film. The strong optical force in the trap not only stably traps the protein molecule but also unfolds it. The unfolding of the BSA is confirmed by experiments with changing optical power and with changing solution pH. The detection of the trapping event has a signal-to-noise ratio of 33, which shows that the setup is extremely sensitive to detect the presence of a protein, even at the single molecule level

    Nanomorphology-Enhanced Gas-Evolution Intensifies CO<sub>2</sub> Reduction Electrochemistry

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    Nanostructured CO<sub>2</sub> reduction catalysts now achieve near-unity reaction selectivity at increasingly improved Tafel slopes and low overpotentials. With excellent surface reaction kinetics, these catalysts encounter CO<sub>2</sub> mass transport limitations at current densities ca. 20 mA cm<sup>–2</sup>. We show here that – in addition to influencing reaction rates and local reactant concentration – the morphology of nanostructured electrodes enhances long-range CO<sub>2</sub> transport via their influence on gas-evolution. Sharper needle morphologies can nucleate and release bubbles as small as 20 μm, leading to a 4-fold increase in the limiting current density compared to a nanoparticle-based catalyst alone. By extending this observation into a diffusion model that accounts for bubble-induced mass transport near the electrode’s surface, diffusive transport can be directly linked to current densities and operating conditions, identifying efficient routes to >100 mA cm<sup>–2</sup> production. We further extend this model to study the influence of mass transport on achieving simultaneously high selectivity and current density of C2 reduction products, identifying precise control of the local fluid environment as a crucial step necessary for producing C2 over C1 products

    Nanomorphology-Enhanced Gas-Evolution Intensifies CO<sub>2</sub> Reduction Electrochemistry

    No full text
    Nanostructured CO<sub>2</sub> reduction catalysts now achieve near-unity reaction selectivity at increasingly improved Tafel slopes and low overpotentials. With excellent surface reaction kinetics, these catalysts encounter CO<sub>2</sub> mass transport limitations at current densities ca. 20 mA cm<sup>–2</sup>. We show here that – in addition to influencing reaction rates and local reactant concentration – the morphology of nanostructured electrodes enhances long-range CO<sub>2</sub> transport via their influence on gas-evolution. Sharper needle morphologies can nucleate and release bubbles as small as 20 μm, leading to a 4-fold increase in the limiting current density compared to a nanoparticle-based catalyst alone. By extending this observation into a diffusion model that accounts for bubble-induced mass transport near the electrode’s surface, diffusive transport can be directly linked to current densities and operating conditions, identifying efficient routes to >100 mA cm<sup>–2</sup> production. We further extend this model to study the influence of mass transport on achieving simultaneously high selectivity and current density of C2 reduction products, identifying precise control of the local fluid environment as a crucial step necessary for producing C2 over C1 products

    Nanomorphology-Enhanced Gas-Evolution Intensifies CO<sub>2</sub> Reduction Electrochemistry

    No full text
    Nanostructured CO<sub>2</sub> reduction catalysts now achieve near-unity reaction selectivity at increasingly improved Tafel slopes and low overpotentials. With excellent surface reaction kinetics, these catalysts encounter CO<sub>2</sub> mass transport limitations at current densities ca. 20 mA cm<sup>–2</sup>. We show here that – in addition to influencing reaction rates and local reactant concentration – the morphology of nanostructured electrodes enhances long-range CO<sub>2</sub> transport via their influence on gas-evolution. Sharper needle morphologies can nucleate and release bubbles as small as 20 μm, leading to a 4-fold increase in the limiting current density compared to a nanoparticle-based catalyst alone. By extending this observation into a diffusion model that accounts for bubble-induced mass transport near the electrode’s surface, diffusive transport can be directly linked to current densities and operating conditions, identifying efficient routes to >100 mA cm<sup>–2</sup> production. We further extend this model to study the influence of mass transport on achieving simultaneously high selectivity and current density of C2 reduction products, identifying precise control of the local fluid environment as a crucial step necessary for producing C2 over C1 products

    Nanomorphology-Enhanced Gas-Evolution Intensifies CO<sub>2</sub> Reduction Electrochemistry

    No full text
    Nanostructured CO<sub>2</sub> reduction catalysts now achieve near-unity reaction selectivity at increasingly improved Tafel slopes and low overpotentials. With excellent surface reaction kinetics, these catalysts encounter CO<sub>2</sub> mass transport limitations at current densities ca. 20 mA cm<sup>–2</sup>. We show here that – in addition to influencing reaction rates and local reactant concentration – the morphology of nanostructured electrodes enhances long-range CO<sub>2</sub> transport via their influence on gas-evolution. Sharper needle morphologies can nucleate and release bubbles as small as 20 μm, leading to a 4-fold increase in the limiting current density compared to a nanoparticle-based catalyst alone. By extending this observation into a diffusion model that accounts for bubble-induced mass transport near the electrode’s surface, diffusive transport can be directly linked to current densities and operating conditions, identifying efficient routes to >100 mA cm<sup>–2</sup> production. We further extend this model to study the influence of mass transport on achieving simultaneously high selectivity and current density of C2 reduction products, identifying precise control of the local fluid environment as a crucial step necessary for producing C2 over C1 products

    Nanomorphology-Enhanced Gas-Evolution Intensifies CO<sub>2</sub> Reduction Electrochemistry

    No full text
    Nanostructured CO<sub>2</sub> reduction catalysts now achieve near-unity reaction selectivity at increasingly improved Tafel slopes and low overpotentials. With excellent surface reaction kinetics, these catalysts encounter CO<sub>2</sub> mass transport limitations at current densities ca. 20 mA cm<sup>–2</sup>. We show here that – in addition to influencing reaction rates and local reactant concentration – the morphology of nanostructured electrodes enhances long-range CO<sub>2</sub> transport via their influence on gas-evolution. Sharper needle morphologies can nucleate and release bubbles as small as 20 μm, leading to a 4-fold increase in the limiting current density compared to a nanoparticle-based catalyst alone. By extending this observation into a diffusion model that accounts for bubble-induced mass transport near the electrode’s surface, diffusive transport can be directly linked to current densities and operating conditions, identifying efficient routes to >100 mA cm<sup>–2</sup> production. We further extend this model to study the influence of mass transport on achieving simultaneously high selectivity and current density of C2 reduction products, identifying precise control of the local fluid environment as a crucial step necessary for producing C2 over C1 products

    High-Density Nanosharp Microstructures Enable Efficient CO<sub>2</sub> Electroreduction

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    Conversion of CO<sub>2</sub> to CO powered by renewable electricity not only reduces CO<sub>2</sub> pollution but also is a means to store renewable energy via chemical production of fuels from CO. However, the kinetics of this reaction are slow due its large energetic barrier. We have recently reported CO<sub>2</sub> reduction that is considerably enhanced via local electric field concentration at the tips of sharp gold nanostructures. The high local electric field enhances CO<sub>2</sub> concentration at the catalytic active sites, lowering the activation barrier. Here we engineer the nucleation and growth of next-generation Au nanostructures. The electroplating overpotential was manipulated to generate an appreciably increased density of honed nanoneedles. Using this approach, we report the first application of sequential electrodeposition to increase the density of sharp tips in CO<sub>2</sub> electroreduction. Selective regions of the primary nanoneedles are passivated using a thiol SAM (self-assembled monolayer), and then growth is concentrated atop the uncovered high-energy planes, providing new nucleation sites that ultimately lead to an increase in the density of the nanosharp structures. The two-step process leads to a new record in CO<sub>2</sub> to CO reduction, with a geometric current density of 38 mA/cm<sup>2</sup> at −0.4 V (vs reversible hydrogen electrode), and a 15-fold improvement over the best prior reports of electrochemical surface area (ECSA) normalized current density

    Longitudinal association of DNA methylation with type 2 diabetes and glycemic traits: A 5-year cross-lagged twin study

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    Previous cross-sectional Epigenome-Wide Association Studies (EWASs) in adults have reported hundreds of 5′-cytosine-phosphate-guanine-3′ (CpG) sites associated with type 2 diabetes mellitus (T2DM) and glycemic traits. However, the results from EWASs have been inconsistent, and longitudinal observations of these associations are scarce. Furthermore, few studies have investigated whether DNAm could be modified by smoking, drinking and glycemic traits, which have broad impacts on genome-wide DNAm, and results in altering the risk of T2DM. Twin studies provide a valuable tool for epigenetic studies, as they are naturally matched for genetic information. In this study, we conducted a systematic literature search in PubMed and EMBASE for EWASs, and 214, 33, and 117 candidate CpG sites were selected for T2DM, HbA1c and fasting blood glucose (FBG). Based on 1,070 twins from the Chinese National Twin Registry, 67, 17 and 16 CpG sites from previous studies were validated for T2DM, HbA1c and FBG. Longitudinal review and blood sampling for phenotypic information and DNAm were conducted twice in 2013 and 2018 on 308 twins. A cross-lagged analysis was performed to examine the temporal relationship between DNAm and T2DM or glycemic traits in the longitudinal data. 11 significant paths from T2DM to subsequent DNAm and 15 paths from DNAm to subsequent T2DM were detected, suggesting both directions of associations. For glycemic traits, we detected 17 cross-lagged associations from baseline glycemic traits to subsequent DNAm, and none was from the other cross-lagged direction, indicating CpG sites may be the consequences, not the causes, of glycemic traits. Finally, a longitudinal mediation analysis was performed to explore the mediation effects of DNAm on the associations of smoking, drinking and glycemic traits with T2DM. No significant mediations of DNAm in the associations linking smoking and drinking with T2DM were found. In contrast, our study suggested the potential role of DNAm of cg19693031, cg00574958 and cg04816311 in mediating the effect of altered glycemic traits on T2DM.</p

    Metabolic and lifestyle risk factors for acute pancreatitis in Chinese adults: A prospective cohort study of 0.5 million people

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    <div><p>Background</p><p>Little prospective evidence exists about risk factors and prognosis of acute pancreatitis in China. We examined the associations of certain metabolic and lifestyle factors with risk of acute pancreatitis in Chinese adults.</p><p>Methods and findings</p><p>The prospective China Kadoorie Biobank (CKB) recruited 512,891 adults aged 30 to 79 years from 5 urban and 5 rural areas between 25 June 2004 and 15 July 2008. During 9.2 years of follow-up (to 1 January 2015), 1,079 cases of acute pancreatitis were recorded. Cox regression was used to estimate adjusted hazard ratios (HRs) for acute pancreatitis associated with various metabolic and lifestyle factors among all or male (for smoking and alcohol drinking) participants. Overall, the mean waist circumference (WC) was 82.1 cm (SD 9.8) cm in men and 79.0 cm (SD 9.5) cm in women, 6% had diabetes, and 6% had gallbladder disease at baseline. WC was positively associated with risk of acute pancreatitis, with an adjusted HR of 1.35 (95% CI 1.27–1.43; <i>p</i> < 0.001) per 1-SD-higher WC. Individuals with diabetes or gallbladder disease had HRs of 1.34 (1.07–1.69; <i>p</i> = 0.01) and 2.42 (2.03–2.88; <i>p</i> < 0.001), respectively. Physical activity was inversely associated with risk of acute pancreatitis, with each 4 metabolic equivalent of task (MET) hours per day (MET-h/day) higher physical activity associated with an adjusted HR of 0.95 (0.91–0.99; <i>p</i> = 0.03). Compared with those without any metabolic risk factors (i.e., obesity, diabetes, gallbladder disease, and physical inactivity), the HRs of acute pancreatitis for those with 1, 2, or ≥3 risk factors were 1.61 (1.47–1.76), 2.36 (2.01–2.78), and 3.41 (2.46–4.72), respectively (<i>p</i> < 0.001). Among men, heavy alcohol drinkers (≥420 g/week) had an HR of 1.52 (1.11–2.09; <i>p</i> = 0.04, compared with abstainers), and current regular smokers had an HR of 1.45 (1.28–1.64; <i>p</i> = 0.02, compared with never smokers). Following a diagnosis of acute pancreatitis, there were higher risks of pancreatic cancer (HR = 8.26 [3.42–19.98]; <i>p</i> < 0.001; 13 pancreatic cancer cases) and death (1.53 [1.17–2.01]; <i>p</i> = 0.002; 89 deaths). Other diseases of the pancreas had similar risk factor profiles and prognosis to acute pancreatitis. The main study limitations are ascertainment of pancreatitis using hospital records and residual confounding.</p><p>Conclusions</p><p>In this relatively lean Chinese population, several modifiable metabolic and lifestyle factors were associated with higher risks of acute pancreatitis, and individuals with acute pancreatitis had higher risks of pancreatic cancer and death.</p></div
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