CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhong Wang,Jinzhou Li,Shuang Yuan,Jinshuo Yang,Zhiqiang Jin,Xinjia Tan,Jie Dang,Wangzhong Mu,Guojian Li,Qiang Wang
FeCoNi-based high entropy intermetallic compounds are promising substitutes for noble metal catalysts for hydrogen evolution reaction (HER) and oxygen evolution (OER), while their activity is restricted by the synergistic effect between the elements. In this paper, the theoretical model of FeCoNiMnMoP bifunctional catalyst has been reasonably designed given the volcanic curve of M−H bond energy as a valuable guide for candidate metal elements. Theoretical calculations show that the synergistic effect between multiple sites not only accelerates the electron transfer but also reduces the rate-determining step (RDS) barrier. At the same time, the introduction of Mo also enhances the total density of states and reduces the d-band center, thus optimizing the adsorption and dissociation of intermediates. The experimental results confirm that the theoretical model has excellent catalytic performance. In the alkaline solution, FeCoNiMnMoP‖FeCoNiMnMoP requires only an ultra-low cell voltage of 1.49 V for overall water splitting when the current density is 10 mA cm −2 . In general, novel insights on the effects of intermetallic synergies on water decomposition are provided, which is helpful for the design of bifunctional catalysts based on volcanic diagrams.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
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2024
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IF 7.5
Xingyu Luo,Cheng Xie,Zhefei Zhao,Meiqin Shi,Huajun Zheng
Graphical Volcano plots are highly effective for understanding catalyst mechanisms and rational designing high-performance catalysts, particularly across different metals. However, the understanding of the relationship between different metals and their reaction mechanisms in 5-Hydroxymethylfurfural (HMF) reduction reactions is still limited. In this study, we explore the Gibbs free diagram of HMF reduction reactions on different metal surfaces and construct a volcano plot that connects HMF adsorption energy with the energy barriers of the rate-determining step. This provides a deeper understanding of HMFRR. Our theoretical findings align well with experimental results. Furthermore, we selectively constructed an AgPb bimetal interface based on our volcano plot, which boosted the catalyst activity. DFT calculations revealed that the AgPb bimetal surface effectively adjusts HMF adsorption energy and reduces energy barriers, suggesting that rational designing bimetal catalysts based on volcano plots is efficient. 2,5-bis(hydroxymethyl)furan (BHMF) derived from 5-Hydroxymethylfurfural (HMF) through a hydrogenation process has extensive applications in the production of resins, polymers, and artificial fibers. However, screening out the candidate and then modulating the active site to optimize the catalyst for high yield of BHMF are currently insufficient. In this study, Gibbs free energy diagrams of the reduction of HMF on 13 metals were presented, along with the identification of the rate-determining step (RDS) with the highest reaction barrier for each metal. We attempted to construct a volcano plot for HMFRR reaction. Additionally, a strategy was proposed to adjust the reaction barriers of RDS by combining two appropriate metals. Further experiments confirmed that Pb with the lowest energy barrier exhibited the highest HMF conversion (BHMF selectivity) among single metals. The modified catalyst by doping Ag on Pb, further boosted the HMF conversion (BHMF selectivity) from 42.1 % (59.4 %) to 80.8 % (80.9 %), respectively. These results provide an approach to rationally design and construct the catalyst system for efficient conversion of HMF.
研究领域:
催化化学
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材料科学
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理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
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2024
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IF 3.8
Yamin Liu,Xunjiang Wang,Jiaojiao Wei,Kangning Fu,Yilin Chen,Linnan Li,Zhengtao Wang,Li Yang
The severe respiratory dysfunctions associated with acute lung injury (ALI) and its sequelae have a high morbidity and mortality rate, are multifactorial, and lack a viable treatment. Considering the critical function that amino acids and derivatives play in the genesis of illnesses and the regulation of metabolic processes, monitoring the levels of metabolites associated with amino acids in biological matrices is necessary and interesting to study their pathological mechanisms. Exploring the dynamics of amino acid and derivatives levels and searching for biomarkers provides improved clinical ideas for the diagnosis and treatment of ALI. Therefore, we developed an ultra-high-performance liquid chromatography-electrospray tandem mass spectrometry (UHPLC-MS/MS) method that can simultaneously determine the amino acid and derivatives metabolic levels to study amino acid profiles in different biological samples to facilitate clinical research of ALI. In this study, 48 amino acids and derivatives, including neurotransmitters, polyamines, purines, and other types, were quantified simultaneously in a fast, high-throughput, sensitive, and reliable manner within a 15-minute run time without derivatization. No relevant studies have been reported to quantify these 48 amino acid metabolites in three biological samples simultaneously. Satisfactory linearity (R > 0.995), inter-day and intra-day accuracy (85.17–112.67% and 85.29–111.60%, respectively), inter-day and intra-day precision (RSD < 13.80% and RSD < 12.01%, respectively), matrix effects (81.00%–118.00%), recovery (85.09%–114.65%) and stability (RSD < 14.72%) were all demonstrated by the optimized method's successful validation for all analytes. In addition, the suggested method was effectively implemented in plasma, urine, and lung tissue from normal mice and mice with ALI, with the aim of finding potential biomarkers associated with ALI. Potential biomarkers were screened through multivariate statistical analysis and volcanic map analysis, and the changes of markers in ALI were again identified through heat map analysis and correlation analysis with biochemical indicators, which provided ideas and references for subsequent mechanism studies. Here, the technique created in this work offers a quick and dependable way to perform an integrated analysis of amino acids in a variety of biological materials, which can provide research ideas for understanding the physiopathological state of various diseases.
研究领域:
肺病学
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分析化学
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代谢组学
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临床研究
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生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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