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首页> 外文期刊>Coordination chemistry reviews >Molecular insights for how preferred oxoanions bind to and stabilize, transition-metal nanoclusters: a tridentate, C_3 symmetry, lattice size-matching binding model
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Molecular insights for how preferred oxoanions bind to and stabilize, transition-metal nanoclusters: a tridentate, C_3 symmetry, lattice size-matching binding model

机译：有关优选含氧阴离子如何结合和稳定过渡金属纳米团簇的分子见解：三齿，C_3对称，晶格尺寸匹配的结合模型

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The recent discovery of an anion efficacy series for the formation and stabilization of transition-metal Ir(0)_n nanoclusters, specifically P_2W_(15)Nb_3O_(62)~(9-) ～SiW_9Nb_3O_(40)~(7-) > C_6H_5O_7~(3-) > [-CH_2-CH(CO_2 )-]_n~(n-) ～OAc~- ～P_3O_9~(3-) ～Cl~- ～OH~-—that is, polyoxoanions > citrate~(3-) > other commonly employed nanocluster stabilizing anions, raises the question of what are the underlying factors behind this preferred order of stabilizers? A brief discussion of three relevant nanocluster papers in the literature, plus a concise summary of the relevant interfacial electrochemistry and surface science literature of C_3 symmetry SO_4~(2-) binding to Ir(111) (as well as to Rh(111), Pt(111), Au(111) and Cu(1111)), are presented first as key background for the lattice size-matching model which follows in which tridentate anions coordinate to transition-metal nanocluster surfaces. A table of nanocluster formation and stabilization data for tridentate oxoanion stabilizers is presented, results which allow two fundamental, previously unavailable, important insights (out of 10 total insights): (ⅰ) the premier anionic stabilizers of transition-metal(0) nanoclusters present a tridentate, facial array of oxygen atoms for coordination to the metal(0) surface; and (ⅱ) the preferred tridentate oxoanion stabilizers of nanoclusters are those that have the best match between the ligand O-O and surface Ir-Ir distances, all other factors being equal—that is, there is a previously unappreciated, geometric, anion-to-surface-metal lattice-size-matching component to the best anionic stabilizers of transition-metal nanoclusters. These are the first molecular-level insights for how the to-date premier tridentate, anionic stabilizers of transition-metal nanoclusters achieve their higher level of stabilization—a non-trivial advance since there was a lack previously of molecular-level insights into how transition-metal nanoclusters are stabilized. Four experimentally testable predictions of the C_3 symmetry, lattice size-matching model for nanocluster M(111) surfaces are presented and briefly discussed. One key prediction is that HPO_~(2-) is a heretofore unappreciated simple, effective and readily available stabilizer of Ir(0) and other transition-metal nanoclusters where there is a lattice-size match between the O-O and the surface M-M distances. Recent experimental evidence is summarized revealing that this prediction is, in fact, true—that is, the third key, new finding of this work is (ⅲ) the first rational design of a new nanocluster stabilizer, HPO_4~(2-) , one shown to be as good a stabilizer as the common nanocluster stabilizer citrate~(3-). The C_3 symmetry, lattice size-matching model is significant in seven additional ways which are detailed in the text and summary which follows.
机译：用于过渡金属Ir（0）_n纳米团簇形成和稳定的阴离子功效系列的最新发现，特别是P_2W_（15）Nb_3O_（62）〜（9-）〜SiW_9Nb_3O_（40）〜（7-）> C_6H_5O_7 〜（3-）> [-CH_2-CH（CO_2）-] _ n〜（n-）〜OAc〜-〜P_3O_9〜（3-）〜Cl〜-〜OH〜-，即多氧阴离子>柠檬酸〜（ 3-）其他常用的纳米簇稳定阴离子提出了一个问题，即这种优选的稳定剂顺序背后的潜在因素是什么？简要讨论了文献中的三篇相关的纳米簇论文，并简要概述了与Ir（111）（以及Rh（111）结合的C_3对称SO_4〜（2-）的相关界面电化学和表面科学文献，首先介绍了Pt（111），Au（111）和Cu（1111）作为晶格尺寸匹配模型的关键背景，随后该模型中三齿阴离子与过渡金属纳米簇表面协调。给出了三齿含氧阴离子稳定剂的纳米簇形成和稳定性数据表，其结果提供了两个基本的，以前不可用的重要见解（共10个见解）：（ⅰ）过渡金属（0）纳米簇的主要阴离子稳定剂存在氧原子的三齿面阵列，用于与金属（0）表面配位； （ⅱ）纳米团簇的优选三齿含氧阴离子稳定剂是那些在配体OO和表面Ir-Ir距离之间具有最佳匹配的稳定剂，在所有其他因素都相等的情况下，也就是以前没有认识到的，几何的，阴离子对表面金属晶格尺寸匹配的成分，是过渡金属纳米簇的最佳阴离子稳定剂。这是关于过渡金属纳米团簇的迄今为止最重要的三齿阴离子稳定剂如何达到更高稳定水平的第一个分子水平的见解，这是一个不小的进步，因为以前缺乏关于如何过渡的分子水平的见解。 -金属纳米团簇稳定。提出并简要讨论了C_3对称性，纳米簇M（111）表面的晶格尺寸匹配模型的四个可实验测试的预测。一个关键的预测是，HPO_（2-）是Ir（0）和其他过渡金属纳米团簇的迄今未曾认识到的简单，有效且容易获得的稳定剂，其中O-O与表面M-M距离之间存在晶格大小匹配。总结了最近的实验证据，揭示了这一预测实际上是正确的，也就是说，这项工作的第三个关键发现是（ⅲ）一种新型纳米簇稳定剂HPO_4〜（2-）的第一个合理设计，一个是显示出与常见的纳米簇稳定剂柠檬酸盐（3-）一样好的稳定剂。 C_3对称的晶格大小匹配模型在另外七个方面具有重要意义，这些在以下文本和摘要中进行了详细介绍。

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