双原子二聚体中的不对称双金属杂化引发硝酸盐到氨的电化学降解的自旋转变

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Surface Science Pub Date : 2024-07-14 DOI:10.1016/j.susc.2024.122549
Ming Meng , Tinghui Li
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引用次数: 0

摘要

具有半填充 3d 轨道的双原子二聚体在从硝酸盐到氨的电化学降解过程中表现出极大的优势,因为它们之间的结合相互作用以及反应物和活性位点之间的电子转移都与自旋有关。在这里,我们提出了一种由双金属杂化引起的局部结构畸变,通过在掺氮孔石墨烯上的锰/锰二聚体中植入一个铁原子来调节自旋构型从低到高,从而使锰的磁矩从 0.48 μB 增加到 3.31 μB。同时,在限速步骤中形成的 *NOH 的活化能可降至 0.79 eV,明显低于原始的铁/铁(1.38 eV)和锰/锰(1.12 eV)二聚体。这些发现为通过调节双原子催化剂的自旋构型来提高其反应活性提供了一种有趣的策略。
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Asymmetric dual-metal-hybridization in dual-atom dimers trigger a spin transition for electrochemical degradation from nitrate to ammonia

The dual-atom dimer with half-filled 3d orbital demonstrates a great advantage in electrochemical degradation from nitrate to ammonia, because their binding interaction and electron transfer between reactants and active sites are spin-dependent. Herein, we suggest a local structure distortion caused by a bimetallic hybridization to regulate the spin configuration from low to high by implanting one Fe atom into the Mn/Mn dimer on holey nitrogen-doped graphene, which makes the Mn magnetic moment increase to 3.31 μB from 0.48 μB. Meanwhile, the activation energy of the formed *NOH at rate-limiting step can be decreased to 0.79 eV, which is obviously lower than the pristine Fe/Fe (1.38 eV) and Mn/Mn (1.12 eV) dimers. These findings enlighten an intriguing strategy to enhance the reactive activity of dual-atom catalysts by regulating their spin configuration.

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来源期刊
Surface Science
Surface Science 化学-物理:凝聚态物理
CiteScore
3.30
自引率
5.30%
发文量
137
审稿时长
25 days
期刊介绍: Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.
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