Solution NMR methods for structural and thermodynamic investigation of nanoparticle adsorption equilibria.

Solution NMR methods for structural and thermodynamic investigation of nanoparticle adsorption equilibria.
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DOI:
10.1039/d2na00099g
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发表时间:
2022-06-14
期刊:
影响因子:
4.7
通讯作者:
--
中科院分区:
材料科学3区
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--
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表征纳米颗粒(NP)表面发生的动态过程对于开发新的和更有效的NP催化剂和材料至关重要。因此,大量的研究一直致力于开发技术来表征吸附平衡。近年来,溶液NMR光谱已成为研究配体-NP相互作用的首选工具。事实上,由于其探测交换动力学的能力在很宽的时间尺度与原子分辨率,溶液NMR可以提供结构,动力学和热力学信息的吸附平衡,涉及多个吸附物种和中间状态。在这方面的贡献,我们回顾了溶液NMR方法表征配体-NP相互作用,并提供了实际应用的例子,使用这些方法作为独立的技术。此外,我们说明了几个NMR数据集的综合分析,阐明了在介导的二氧化铈负载的Pd纳米粒子催化的苯酚加氢反应的支持-衬底相互作用所发挥的作用。溶液NMR方法提供了复杂的吸附平衡,涉及多个中间体和吸附物种的结构,热力学和动力学信息。
Characterization of dynamic processes occurring at the nanoparticle (NP) surface is crucial for developing new and more efficient NP catalysts and materials. Thus, a vast amount of research has been dedicated to developing techniques to characterize sorption equilibria. Over recent years, solution NMR spectroscopy has emerged as a preferred tool for investigating ligand–NP interactions. Indeed, due to its ability to probe exchange dynamics over a wide range of timescales with atomic resolution, solution NMR can provide structural, kinetic, and thermodynamic information on sorption equilibria involving multiple adsorbed species and intermediate states. In this contribution, we review solution NMR methods for characterizing ligand–NP interactions, and provide examples of practical applications using these methods as standalone techniques. In addition, we illustrate how the integrated analysis of several NMR datasets was employed to elucidate the role played by support–substrate interactions in mediating the phenol hydrogenation reaction catalyzed by ceria-supported Pd nanoparticles. Solution NMR methods provide structural, thermodynamic, and kinetic information on complex sorption equilibria involving multiple intermediates and adsorbed species.
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