当前位置: X-MOL 学术J. Am. Chem. Soc. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Editorial Summary of the Comment and Responses on “Following Molecular Mobility during Chemical Reactions: No Evidence for Active Propulsion” and “Molecular Diffusivity of Click Reaction Components: The Diffusion Enhancement Question”
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-08-03 , DOI: 10.1021/jacs.2c05873
Lyndon Emsley 1
Affiliation  

The addition of Gd chelates is used in [ (2)] in order to overcome a possible problem of the original study [ (6)], namely that changes in the concentration of paramagnetic species during the reaction might modify the T1 values, which in turn might affect the observed intensities. This effect can be mitigated by adding Gd chelates to the solution, which then dominate the relaxation mechanisms, thereby greatly reducing the relative effect of changing reagent/product concentrations on T1 times. The Comment challenges this procedure on the grounds that the Gd chelates are not chemically inert, and Huang and Granick (1) give evidence to that effect. The Comment also proposes that [ (2)] uses an over-simplified analysis of the PFG diffusion data, which does not account for the effect of transient binding of water and reagents to the paramagnetic complex. Article [ (2)] is also criticized for attributing peak overlap to some of the proposed misinterpretations in [ (6)]. Experimental evidence is advanced to show that peak overlap is not responsible for the reported effects. Article [ (3)] proposes that the reference value for the diffusion coefficients to which comparisons are made is the reagent in D2O in the absence of catalyst, co-catalyst, and the second reagent. The Comment suggests that the correct reference state should be the unreacting mixture (i.e., everything but the copper catalyst). The Comment states that some of the data given in [ (3)] is obtained on mixtures which flocculate, and they provide photographic evidence. This article references 11 other publications. This article has not yet been cited by other publications. This article references 11 other publications.

中文翻译:

关于“在化学反应中跟随分子迁移率:没有证据表明主动推进”和“点击反应组分的分子扩散率:扩散增强问题”的评论和回复的编辑摘要

在 [(2)] 中添加 Gd 螯合物是为了克服原始研究 [(6)] 中可能存在的问题,即反应期间顺磁性物质浓度的变化可能会改变T 1值,这反过来可能会影响观察到的强度。这种影响可以通过向溶液中添加 Gd 螯合物来减轻,然后 Gd 螯合物主导弛豫机制,从而大大降低了改变试剂/产品浓度对T 1的相对影响次。评论以 Gd 螯合物不是化学惰性为由对这一程序提出质疑,Huang 和 Granick (1) 对此提供了证据。评论还建议 [(2)] 对 PFG 扩散数据进行过度简化的分析,这没有考虑水和试剂与顺磁性复合物的瞬时结合的影响。第 [(2)] 条也因将峰值重叠归因于 [(6)] 中提出的一些误解而受到批评。实验证据表明峰重叠不是报告的影响的原因。[(3)]条提出,扩散系数的参考值是D 2中的试剂O 在没有催化剂、助催化剂和第二试剂的情况下。评论建议正确的参考状态应该是未反应的混合物(即,除了铜催化剂之外的所有物质)。评论指出,[(3)] 中给出的一些数据是从絮凝混合物中获得的,它们提供了照片证据。本文引用了其他 11 种出版物。这篇文章尚未被其他出版物引用。本文引用了其他 11 种出版物。
更新日期:2022-08-03
down
wechat
bug