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result(s) for
"Gu, Lin"
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Interstitial boron-triggered electron-deficient Os aerogels for enhanced pH-universal hydrogen evolution
2022
Developing high-performance electrocatalysts for hydrogen evolution reaction (HER) is crucial for sustainable hydrogen production, yet still challenging. Here, we report boron-modulated osmium (B-Os) aerogels with rich defects and ultra-fine diameter as a pH-universal HER electrocatalyst. The catalyst shows the small overpotentials of 12, 19, and 33 mV at a current density of 10 mA cm
−2
in acidic, alkaline, and neutral electrolytes, respectively, as well as excellent stability, surpassing commercial Pt/C. Operando X-ray absorption spectroscopy shows that interventional interstitial B atoms can optimize the electron structure of B-Os aerogels and stabilize Os as active sites in an electron-deficient state under realistic working conditions, and simultaneously reveals the HER catalytic mechanisms of B-Os aerogels in pH-universal electrolytes. The density functional theory calculations also indicate introducing B atoms can tailor the electronic structure of Os, resulting in the reduced water dissociation energy and the improved adsorption/desorption behavior of hydrogen, which synergistically accelerate HER.
While noble metals can be active electrocatalysts for producing renewable H
2
, there are relatively few works examining osmium materials. Here, the authors prepare boron-doped osmium aerogels for H
2
evolution electrocatalysis plus examine the mechanism using computational and in situ characterization.
Journal Article
Ensemble learning for integrative prediction of genetic values with genomic variants
by
Jiang, Dan
,
Gu, Lin-Lin
,
Yang, Run-Qing
in
Algorithms
,
Analysis
,
Big Data and Machine Learning in Bioinformatics and Medical Informatics
2024
Background
Whole genome variants offer sufficient information for genetic prediction of human disease risk, and prediction of animal and plant breeding values. Many sophisticated statistical methods have been developed for enhancing the predictive ability. However, each method has its own advantages and disadvantages, so far, no one method can beat others.
Results
We herein propose an Ensemble Learning method for Prediction of Genetic Values (ELPGV), which assembles predictions from several basic methods such as GBLUP, BayesA, BayesB and BayesCπ, to produce more accurate predictions. We validated ELPGV with a variety of well-known datasets and a serious of simulated datasets. All revealed that ELPGV was able to significantly enhance the predictive ability than any basic methods, for instance, the comparison
p
-value of ELPGV over basic methods were varied from 4.853E−118 to 9.640E−20 for WTCCC dataset.
Conclusions
ELPGV is able to integrate the merit of each method together to produce significantly higher predictive ability than any basic methods and it is simple to implement, fast to run, without using genotype data. is promising for wide application in genetic predictions.
Journal Article
Epidemiology and Immune Pathogenesis of Viral Sepsis
by
Drysdale, Simon B.
,
McGinley, Joseph P.
,
Pollard, Andrew J.
in
Antibiotics
,
Antimicrobial resistance
,
Epidemiology
2018
Sepsis is a life-threatening organ dysfunction caused by a dysregulated host response to infection. Sepsis can be caused by a broad range of pathogens; however, bacterial infections represent the majority of sepsis cases. Up to 42% of sepsis presentations are culture negative, suggesting a non-bacterial cause. Despite this, diagnosis of viral sepsis remains very rare. Almost any virus can cause sepsis in vulnerable patients (e.g., neonates, infants, and other immunosuppressed groups). The prevalence of viral sepsis is not known, nor is there enough information to make an accurate estimate. The initial standard of care for all cases of sepsis, even those that are subsequently proven to be culture negative, is the immediate use of broad-spectrum antibiotics. In the absence of definite diagnostic criteria for viral sepsis, or at least to exclude bacterial sepsis, this inevitably leads to unnecessary antimicrobial use, with associated consequences for antimicrobial resistance, effects on the host microbiome and excess healthcare costs. It is important to understand non-bacterial causes of sepsis so that inappropriate treatment can be minimised, and appropriate treatments can be developed to improve outcomes. In this review, we summarise what is known about viral sepsis, its most common causes, and how the immune responses to severe viral infections can contribute to sepsis. We also discuss strategies to improve our understanding of viral sepsis, and ways we can integrate this new information into effective treatment.
Journal Article
Photochemical route for synthesizing atomically dispersed palladium catalysts
2016
Atomically dispersed noble metal catalysts often exhibit high catalytic performances, but the metal loading density must be kept low (usually below 0.5%) to avoid the formation of metal nanoparticles through sintering. We report a photochemical strategy to fabricate a stable atomically dispersed palladium–titanium oxide catalyst (Pd₁/TiO₂) on ethylene glycolate (EG)–stabilized ultrathin TiO₂ nanosheets containing Pd up to 1.5%. The Pd₁/TiO₂ catalyst exhibited high catalytic activity in hydrogenation of C=C bonds, exceeding that of surface Pd atoms on commercial Pd catalysts by a factor of 9. No decay in the activity was observed for 20 cycles. More important, the Pd₁/TiO₂-EG system could activate H₂ in a heterolytic pathway, leading to a catalytic enhancement in hydrogenation of aldehydes by a factor of more than 55.
Journal Article
Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts
2019
Although single-atomically dispersed metal-N
x
on carbon support (M-NC) has great potential in heterogeneous catalysis, the scalable synthesis of such single-atom catalysts (SACs) with high-loading metal-N
x
is greatly challenging since the loading and single-atomic dispersion have to be balanced at high temperature for forming metal-N
x
. Herein, we develop a general cascade anchoring strategy for the mass production of a series of M-NC SACs with a metal loading up to 12.1 wt%. Systematic investigation reveals that the chelation of metal ions, physical isolation of chelate complex upon high loading, and the binding with N-species at elevated temperature are essential to achieving high-loading M-NC SACs. As a demonstration, high-loading Fe-NC SAC shows superior electrocatalytic performance for O
2
reduction and Ni-NC SAC exhibits high electrocatalytic activity for CO
2
reduction. The strategy paves a universal way to produce stable M-NC SAC with high-density metal-N
x
sites for diverse high-performance applications.
Although single atom catalysts (SACs) with high-loading metal-Nx have great potential in heterogeneous catalysis, their scalable synthesis remains challenging. Here, the authors develop a general cascade anchoring strategy for the mass production of a series of metal-Nx SACs with a metal loading up to 12.1 wt%.
Journal Article
Electrochemically activated spinel manganese oxide for rechargeable aqueous aluminum battery
2019
Aluminum is a naturally abundant, trivalent charge carrier with high theoretical specific capacity and volumetric energy density, rendering aluminum-ion batteries a technology of choice for future large-scale energy storage. However, the frequent collapse of the host structure of the cathode materials and sluggish kinetics of aluminum ion diffusion have thus far hampered the realization of practical battery devices. Here, we synthesize Al
x
MnO
2
·
n
H
2
O by an in-situ electrochemical transformation reaction to be used as a cathode material for an aluminum-ion battery with a configuration of Al/Al(OTF)
3
-H
2
O/Al
x
MnO
2
·
n
H
2
O. This cell is not only based on aqueous electrolyte chemistry but also delivers a high specific capacity of 467 mAh g
−1
and a record high energy density of 481 Wh kg
−1
. The high safety of aqueous electrolyte, facile cell assembly and the low cost of materials suggest that this aqueous aluminum-ion battery holds promise for large-scale energy applications.
The instability of the host structure of cathode materials and sluggish aluminium ion diffusion are the major challenges facing the Al-ion battery. Here the authors show Al
x
MnO
2
·
n
H
2
O as a cathode that allows for reversible Al
3+
(de)intercalation in an aqueous electrolyte and impressive electrochemical performance for a battery device.
Journal Article
Metabolic Syndrome and Psoriasis: Mechanisms and Future Directions
2021
Psoriasis is an immune-mediated systemic disease with associated comorbidities, including metabolic syndrome (MetS) which contributes substantially to premature mortality in patients with psoriasis. However, the pathological mechanisms underlying this comorbidity are unclear. Studies have shown that the pathological parameters of psoriasis mediate the development of MetS. We reviewed the potential mechanisms which mediate the association between psoriasis and MetS, including endoplasmic reticulum stress, pro-inflammatory cytokine releases, excess production of reactive oxygen species, alterations in adipocytokine levels and gut microbiota dysbiosis. Here, we highlight important research questions regarding this association and offer insights into MetS research and treatment.
Journal Article
A universal ligand mediated method for large scale synthesis of transition metal single atom catalysts
2019
There is interest in metal single atom catalysts due to their remarkable activity and stability. However, the synthesis of metal single atom catalysts remains somewhat ad hoc, with no universal strategy yet reported that allows their generic synthesis. Herein, we report a universal synthetic strategy that allows the synthesis of transition metal single atom catalysts containing Cr, Mn, Fe, Co, Ni, Cu, Zn, Ru, Pt or combinations thereof. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure spectroscopy confirm that the transition metal atoms are uniformly dispersed over a carbon black support. The introduced synthetic method allows the production of carbon-supported metal single atom catalysts in large quantities (>1 kg scale) with high metal loadings. A Ni single atom catalyst exhibits outstanding activity for electrochemical reduction of carbon dioxide to carbon monoxide, achieving a 98.9% Faradaic efficiency at −1.2 V.
Single-atom catalysts are a promising class of catalytic materials, but general synthetic methods are limited. Here, the authors develop a ligand-mediated strategy that allows the large-scale synthesis of diverse transition metal single atom catalysts supported on carbon.
Journal Article
Cobalt carbide nanoprisms for direct production of lower olefins from syngas
2016
Lower olefins are hydrocarbons that are widely used in the chemical industry, and can be generated from syngas by the ‘Fischer–Tropsch to olefins’ process; here, a new catalyst is described that can generate lower olefins from syngas with high selectivity, with little formation of undesirable methane.
Lower olefines—and not much methane—from biomass
The lower olefins—chiefly ethylene, propylene and butylene—are starting materials for many plastics and other industrial products. They are usually obtained by cracking hydrocarbon feedstocks, so as petroleum reserves become depleted the urgency to switch to alternative feedstocks such as biomass increases. The 'Fischer–Tropsch to olefins' (FTO) process produces lower olefines from syngas—a mixture of hydrogen and carbon monoxide derived from biomass, coal and natural gas—but at the same time produces large amounts of unwanted methane. Here Liangshu Zhong and colleagues describe a new catalyst for the FTO conversion. Formed from cobalt carbide nanoprisms, the catalyst is active in mild reaction conditions, is highly selective for lower olefins and, critically, produces very little methane.
Lower olefins—generally referring to ethylene, propylene and butylene—are basic carbon-based building blocks that are widely used in the chemical industry, and are traditionally produced through thermal or catalytic cracking of a range of hydrocarbon feedstocks, such as naphtha, gas oil, condensates and light alkanes
1
,
2
. With the rapid depletion of the limited petroleum reserves that serve as the source of these hydrocarbons, there is an urgent need for processes that can produce lower olefins from alternative feedstocks
3
,
4
,
5
,
6
,
7
,
8
,
9
. The ‘Fischer–Tropsch to olefins’ (FTO) process has long offered a way of producing lower olefins directly from syngas—a mixture of hydrogen and carbon monoxide that is readily derived from coal, biomass and natural gas
3
,
4
,
5
,
6
,
7
. But the hydrocarbons obtained with the FTO process typically follow the so-called Anderson–Schulz–Flory distribution, which is characterized by a maximum C
2
–C
4
hydrocarbon fraction of about 56.7 per cent and an undesired methane fraction of about 29.2 per cent (refs
1
,
10
,
11
,
12
). Here we show that, under mild reaction conditions, cobalt carbide quadrangular nanoprisms catalyse the FTO conversion of syngas with high selectivity for the production of lower olefins (constituting around 60.8 per cent of the carbon products), while generating little methane (about 5.0 per cent), with the ratio of desired unsaturated hydrocarbons to less valuable saturated hydrocarbons amongst the C
2
–C
4
products being as high as 30. Detailed catalyst characterization during the initial reaction stage and theoretical calculations indicate that preferentially exposed {101} and {020} facets play a pivotal role during syngas conversion, in that they favour olefin production and inhibit methane formation, and thereby render cobalt carbide nanoprisms a promising new catalyst system for directly converting syngas into lower olefins.
Journal Article
Ultrahigh–energy density lead-free dielectric films via polymorphic nanodomain design
2019
Dielectric capacitors with ultrahigh power densities are fundamental energy storage components in electrical and electronic systems. However, a long-standing challenge is improving their energy densities. We report dielectrics with ultrahigh energy densities designed with polymorphic nanodomains. Guided by phase-field simulations, we conceived and synthesized lead-free BiFeO₃-BaTiO₃-SrTiO₃ solid-solution films to realize the coexistence of rhombohedral and tetragonal nanodomains embedded in a cubic matrix. We obtained minimized hysteresis while maintaining high polarization and achieved a high energy density of 112 joules per cubic centimeter with a high energy efficiency of ~80%. This approach should be generalizable for designing high-performance dielectrics and other functional materials that benefit from nanoscale domain structure manipulation.
Journal Article