CAS:Mechanistic Investigation of Heme-based Catalysts for Sustainable Carbene Transfer Reactions

CAS:可持续卡宾转移反应的血红素基催化剂的机理研究

基本信息

  • 批准号:
    2054897
  • 负责人:
  • 金额:
    $ 36万
  • 依托单位:
  • 依托单位国家:
    美国
  • 项目类别:
    Standard Grant
  • 财政年份:
    2021
  • 资助国家:
    美国
  • 起止时间:
    2021-06-01 至 2025-05-31
  • 项目状态:
    未结题

项目摘要

With support from the Chemical Catalysis program in the Division of Chemistry, Dr. Yong Zhang of Stevens Institute of Technology will conduct a rigorous computational study to improve catalyst design for selected important transformations in sustainable chemistry. The targeted catalysts are engineered heme proteins with numerous attractive properties, such as delivering products in high yield, with high chemo-, regio-, and stereoselectivity, at room temperature, in aqueous solution, with biocompatibility and low toxicity. These catalysts also incorporate the most abundant and least expensive transition metal, Fe (iron). That said, big challenges for certain catalytic transformations involved in synthesis of natural products, drugs, and biological compounds still persist, in particular regarding the reactions of cyclopropanation and nitrogen-hydrogen insertion, particularly if one is to rely upon Fe-catalysis. Dr. Zhang’s research group employs high accuracy computational techniques to provide the previously unknown mechanistic information of such heme-based catalysts. In particular, Dr. Zhang will work toward enhancing their catalytic reactivity and selectivity for these challenging chemical transformations. Such insights may lead to improvements in certain process chemistry procedures conducted on scale in the pharmaceutical industry, for example. Dr. Zhang’s research is broadly integrated with teaching, training, and learning, with broad participation of students from different groups at various levels, particularly those from underrepresented groups. Several channels are employed to broadly disseminate their research results to the community. For example, students in this NSF-supported project give presentations/reports in their classes, and within their department and/or university. There are also outreach programs for K-12 institutions, museums, news media (both traditional mass media and social media), enhancing the scientific understanding of the impacts of this project. Cyclopropanation is useful for synthesis of natural products and pharmaceutical compounds and N-H insertion is useful for synthesis of amino acids, alkaloids, N-heterocyclic compounds, and bioconjugation. Engineered heme proteins have exhibited numerous excellent catalytic properties for sustainable carbene transfer reactions. Yet there are still some big challenges for certain catalytic cyclopropanations and N-H insertions, particularly for electron-poor substrates. The origins of varied cyclopropanation vs. N-H insertion chemoselectivity in some experimental systems are also unknown. Dr. Yong Zhang’s research group is conducting a rigorous quantum chemical computational study of the previously unknown mechanistic details of some heme structural factors toward enhancing catalytic reactivities for challenging cyclopropanations and N-H insertions. Insights into variable cyclopropanation vs. N-H insertion chemoselectivity from different catalyst components are sought to help design 'matched ' catalysts for selective functionalization. Dr. Zhang’s research is broadly integrated with teaching, training, and learning. Students in his lab are actively involved in classes and outreach programs that incorporate their research results. Dr. Zhang continues his vigorous efforts to have broad participation of students from diverse groups at various levels, particularly including students from underrepresented groups. Several channels are employed by Dr. Zhang’s research group to broadly disseminate their research results to the scientific community and general public.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.
在化学系化学催化项目的支持下,史蒂文斯理工学院的张勇博士将进行严格的计算研究,以改进可持续化学中选定的重要转化的催化剂设计。目标催化剂是具有众多吸引力的工程血红素蛋白。这些催化剂还包含最丰富且最便宜的过渡金属 Fe,例如在室温下、在水溶液中以高产率、高化学选择性、区域选择性和立体选择性提供产物,并具有生物相容性和低毒性。也就是说,天然产物、药物和生物化合物合成中涉及的某些催化转化仍然存在巨大挑战,特别是在环丙烷化和氮氢插入反应方面,特别是如果要依赖 Fe-。张博士的研究小组采用高精度计算技术来提供此类基于血红素的催化剂的先前未知的机理信息,张博士将致力于提高这些具有挑战性的化学品的催化反应活性和选择性。这些转变可能会导致制药行业大规模实施的某些工艺化学程序的改进,例如,张博士的研究广泛地与教学、培训和学习相结合,并得到了来自不同层次的不同群体的学生的广泛参与。 ,特别是那些来自代表性不足的群体。例如,这个 NSF 支持的项目的学生在他们的班级以及他们的部门和/或大学内进行演讲/报告。还有外展计划K-12 机构、博物馆、新闻媒体(传统大众媒体和社交媒体),增强对该项目影响的科学理解。环丙烷化有助于合成天然产物和药物化合物,N-H 插入有助于合成氨基。酸、生物碱、N-杂环化合物和生物共轭蛋白在可持续的卡宾转移反应中表现出许多优异的催化特性,但某些催化仍然存在一些巨大的挑战。环丙烷化和 N-H 插入,特别是对于缺电子底物 在一些实验系统中,各种环丙烷化与 N-H 插入化学选择性的起源也是未知的。 张勇博士的研究小组正在对以前未知的机制细节进行严格的量子化学计算研究。一些血红素结构因素,以增强具有挑战性的环丙烷化和 N-H 插入的催化反应性 深入了解可变环丙烷化与 N-H 插入。不同催化剂组分的化学选择性有助于设计用于选择性功能化的“匹配”催化剂。张博士的研究广泛地与教学、培训和学习相结合。他的实验室的学生积极参与课堂推广和融入其研究成果的项目。张博士继续积极努力让来自不同层次的不同群体的学生,特别是来自代表性不足群体的学生广泛参与。张博士的研究小组利用多种渠道向科学界和公众广泛传播他们的研究成果。该奖项反映了 NSF 的法定使命,并通过使用基金会的智力价值和更广泛的影响审查标准进行评估,被认为值得支持。

项目成果

期刊论文数量(5)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Liposome‐Templated Green Synthesis of Mesoporous Metal Nanostructures with Universal Composition for Biomedical Application
脂质体——生物医学应用通用组合物介孔金属纳米结构的模板绿色合成
  • DOI:
    10.1002/smll.202304880
  • 发表时间:
    2023-07
  • 期刊:
  • 影响因子:
    13.3
  • 作者:
    Wang, Jinping;Sun, Jingyu;Khade, Rahul L.;Chou, Tsengming;An, Hailong;Zhang, Yong;Wang, Hongjun
  • 通讯作者:
    Wang, Hongjun
Generation and Application of Homoallylic α,α‐Diboryl Radicals via Diboron‐Promoted Ring‐Opening of Vinyl Cyclopropanes: cis ‐Diastereoselective Borylative Cycloaddition**
通过二硼生成和应用同烯丙基 α,α-二硼基自由基-促进环-乙烯基环丙烷的开环:顺式-非对映选择性硼基环加成**
  • DOI:
    10.1002/chem.202303175
  • 发表时间:
    2023-11
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Vyas, Het;Gangani, Ashvin J.;Mini, Aiswarya;Lin, Shengjia;Chu, Jia‐Min;Agee, Caitlyn O.;Gabriel, Justin;Williamson, R. Thomas;Zhang, Yong;Sharma, Abhishek
  • 通讯作者:
    Sharma, Abhishek
Biocatalytic Intramolecular C−H aminations via Engineered Heme Proteins: Full Reaction Pathways and Axial Ligand Effects
通过工程血红素蛋白进行生物催化分子内 C–H 胺化:完整反应途径和轴向配体效应
  • DOI:
    10.1002/chem.202202006
  • 发表时间:
    2022-08
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Wei, Yang;Conklin, Melissa;Zhang, Yong
  • 通讯作者:
    Zhang, Yong
Computational Mechanistic Investigations of Biocatalytic Nitrenoid C−H Functionalizations via Engineered Heme Proteins
通过工程血红素蛋白生物催化类氮化合物 C–H 功能化的计算机制研究
  • DOI:
    10.1002/cbic.202300260
  • 发表时间:
    2023-07
  • 期刊:
  • 影响因子:
    3.2
  • 作者:
    Zhang, Yong;Chu, Jia‐Min
  • 通讯作者:
    Chu, Jia‐Min
Mechanistic manifold in a hemoprotein-catalyzed cyclopropanation reaction with diazoketone
血红素蛋白催化的重氮酮环丙烷化反应的机理
  • DOI:
    10.1038/s41467-023-43559-7
  • 发表时间:
    2023-12-02
  • 期刊:
  • 影响因子:
    16.6
  • 作者:
    Nam, Donggeon;Bacik, John-Paul;Khade, Rahul L.;Aguilera, Maria Camila;Wei, Yang;Villada, Juan D.;Neidig, Michael L.;Zhang, Yong;Ando, Nozomi;Fasan, Rudi
  • 通讯作者:
    Fasan, Rudi
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Yong Zhang其他文献

Effects of pterostilbene on treating hyperprolactinemia and related mechanisms.
紫檀芪治疗高催乳素血症的作用及相关机制。
Quality Prediction of Rocket Engine Combustion Chamber Shell Spinning Process Based on CGAN and Hybrid Neural Network
基于CGAN和混合神经网络的火箭发动机燃烧室壳体旋压过程质量预测
  • DOI:
    10.1109/cac59555.2023.10451579
  • 发表时间:
    2023-11-17
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Junbo Yi;Xin He;Maolin Wang;Xiujuan Zheng;Feng Guo;Yong Zhang
  • 通讯作者:
    Yong Zhang
Parameterized Approximation Algorithms for Sum of Radii Clustering and Variants
半径聚类和变体之和的参数化近似算法
  • DOI:
    10.1609/aaai.v38i18.30053
  • 发表时间:
    2024-03-24
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Xianrun Chen;Dachuan Xu;Yicheng Xu;Yong Zhang
  • 通讯作者:
    Yong Zhang
Low temperature preparation and superconductivity of F-doped SmFeAsO
F掺杂SmFeAsO的低温制备及超导
  • DOI:
    10.1016/j.physc.2010.05.017
  • 发表时间:
    2010-11-01
  • 期刊:
  • 影响因子:
    1.7
  • 作者:
    Yongliang Chen;Y. Cui;C. H. Cheng;Ye Yang;Lulin Wang;Yuhang Li;Yong Zhang;Yong Zhao
  • 通讯作者:
    Yong Zhao
Generation and application of immortalized sertoli cell line from sheep testis.
绵羊睾丸永生化支持细胞系的产生及应用
  • DOI:
    10.1016/j.jviromet.2023.114727
  • 发表时间:
    2023-03-01
  • 期刊:
  • 影响因子:
    3.1
  • 作者:
    Guoyu Du;Jinyan Wu;Cheng Zhang;Xiaoan Cao;Lingxia Li;Jijun He;Yong Zhang;Y. Shang
  • 通讯作者:
    Y. Shang

Yong Zhang的其他文献

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{{ truncateString('Yong Zhang', 18)}}的其他基金

CMG Collaborative Research: Tempered Stable Models for Preasymptotic Pollutant Transport in Natural Media
CMG 合作研究:自然介质中渐进前污染物传输的稳定模型
  • 批准号:
    1460319
  • 财政年份:
    2014
  • 资助金额:
    $ 36万
  • 项目类别:
    Standard Grant
SusChEM: Selective C-H Functionalization by Highly Tunable Metalloporphyrin Carbenoid: A Mechanistic Investigation
SusChEM:高度可调金属卟啉类胡萝卜素选择性 C-H 官能化:机理研究
  • 批准号:
    1300912
  • 财政年份:
    2013
  • 资助金额:
    $ 36万
  • 项目类别:
    Continuing Grant
CMG Collaborative Research: Tempered Stable Models for Preasymptotic Pollutant Transport in Natural Media
CMG 合作研究:自然介质中渐进前污染物传输的稳定模型
  • 批准号:
    1025417
  • 财政年份:
    2010
  • 资助金额:
    $ 36万
  • 项目类别:
    Standard Grant
Collaborative Research: A Comparison of Local and Nonlocal Transport Theories
合作研究:本地和非本地运输理论的比较
  • 批准号:
    0748953
  • 财政年份:
    2007
  • 资助金额:
    $ 36万
  • 项目类别:
    Standard Grant

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Mechanistic links between mutations in the CLPB gene and congenital neutropenia
CLPB基因突变与先天性中性粒细胞减少症之间的机制联系
  • 批准号:
    10526864
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iPSC 衍生的显性 LCA 模型的机制分析和等位基因组编辑
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Therapeutic and Mechanistic Evaluation of Cannabis sativa Terpenes in Neuropathic Pain
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