CATALYZED AMIDE ISOMERIZATION: SYNTHETIC ROTAMASES
CATALYZED AMIDE ISOMERIZATION: SYNTHETIC ROTAMASES
批准号:
2655017
负责人:
THOMAS C. LECTKA
金额:
$9.64万
依托单位:
依托单位国家:
美国
项目类别:
财政年份:
1997
资助国家:
美国
项目状态:
已结题
起止时间:
1997-02-01 至 2002-01-31
中文摘要
这项提议的目的是消除温和的、有选择性的
用于酰胺异构化(AI)的催化剂,最终在系统
催化多肽折叠的模型酶--轮转酶的研究进展
通过脯氨酸残基的顺反异构化。PI表示
反过来,他提出了针对不同个体方面的实验
指包括金属离子催化在内的酶催化;由
去溶解;扭曲催化;自催化,最后他
将这些不同的概念整合到一个建议中,以合成
使用分子印迹策略的木聚糖酶,其中合成的
模板分子或“半抗原”以非共价方式与一种修饰的
交联剂,然后与模板组件共聚
适用于生产高度CROS连接的大孔聚合物和
模板分子被移除,以使Beha=ind刚性空腔能够
识别在形状上与模板相似的酰胺,或更多
识别在形状上与模板相似的酰胺,或更多
微妙地,氢键供体或受体的能力。值得注意的是,由于
模板被设计为接近模拟AI的过渡状态
(尤其是脯氨酸异构化),聚合物将完全作为
合成的谷氨酰胺酶。
初步数据包括第一批记录的金属离子催化案例。
AI,在温和的条件下使用亚化学计量的金属;
一般酸催化的人工智能;模型系统中的自催化;以及
胶束催化的人工智能,它第一次模拟了
酶法去溶对木聚糖酶活性的影响。私家侦探注意到他的初选
目标是详细了解决定因素的各种复杂因素
将他的初步结果应用于有机中的问题
合成,并催化日益复杂的体系的折叠
包括多肽,最终是蛋白质。他建议除了
本研究将对轮胺酶催化的基本认识
帮助实现,实际应用包括小说的开发
对映体选择性变形。
英文摘要
DESCRIPTION; The goal of this proposal is to disvover mild, selective
catalysts for amide isomerization (AI), culminating in the systematic
development of model rotamase enzymes that catalyze the folding of peptides
through the cis-trans isomerization of proline residues. The PI indicates
that in turn he proposes experiments that address various individual facets
of rotamase catalysis, including metal iion catalysis; catalysis by
desolvation; catalysis by distortion; and autocatalysis and that finally he
integrates these diverse concepts together into a proposal for synthetic
rotamases using the strategy of molecular imprintation, wherein a synthetic
template molecule, or "hapten", is complexed non-covalently with a modified
crosslinking reagent, the template assemblies are then copolymerized with
suitable nomomers to produce highly cros-linked, macroporous polymers and
template molecules are removed to leave beha=ind rigid cavities able to
recognize amides which resemble the template in terms of shape, or more
recognize amides which resemble the template in terms of shape, or more
subtly, hydrogen bond donor or acceptor ability. It is noted that since the
template is designed to closely mimic the transition state for AI
(especially proline isomerization), the polymer would serve as a totally
synthetic rotamase enzyme.
Preliminary data include the first documented cases of metal ion catalyzed
AI, employing substoichiometric amounts of metal under mild conditions;
general acid-catalyzed AI; autocatalysis in model systems; and
miceelle-catalyzed AI, which for the first tiem models the effects of
enzymatic desolvation on rotamase activity. The PI notes that his primary
objective is to understand in detail the various complex factors dictating
rotamase catalysis, to apply his preliminary results to problems in organic
synthesis, and to catalyze the folding of increasingly complex systems
including polypeptides and eventually proteins. He suggests that aside from
the fundamental understanding of rotamase catalysis that this study will
help achieve, practical applications include the development of novel
enantioselective transformaitons.
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