Real-time insight into the multistage mechanism of nanoparticle exsolution from a perovskite host surface.
Real-time insight into the multistage mechanism of nanoparticle exsolution from a perovskite host surface.
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DOI：
10.1038/s41467-023-37212-6
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发表时间：
2023-03-29
影响因子：
16.6
通讯作者：
Payne, David J.
中科院分区：
文献类型：
--
作者：
Cali, Eleonora;Thomas, Melonie P.;Vasudevan, Rama;Wu, Ji;Gavalda-Diaz, Oriol;Marquardt, Katharina;Saiz, Eduardo;Neagu, Dragos;Unocic, Raymond R.;Parker, Stephen C.;Guiton, Beth S.;Payne, David J.
在溶液外，纳米粒子通过氧化还原驱动力从氧化物主体中涌出，导致稳定性、活性和效率方面的变革性进步，超过了沉积技术，并为催化、能源和净零相关技术带来了广泛的新机会。然而，到目前为止，纳米颗粒成核和钙钛矿结构演变的机制仍然不清楚。在这里，我们通过使用高分辨率电子显微镜结合计算模拟和机器学习分析，实时跟踪从SrTiO_3基质氧化物晶格中出现的Ir纳米颗粒来阐明这一难以捉摸的过程。我们发现成核是通过原子簇合的方式进行的，同时伴随着主体的演化，揭示了表面缺陷和主体晶格重构参与了捕获Ir原子的过程，从而启动了纳米粒子的形成和生长。这些见解为进一步开发高功能和广泛适用的可溶材料提供了理论平台和实践建议。通过出溶将纳米颗粒从氧化物主体中分离出来，形成了催化和能源相关应用的基础。在这里，作者结合实时电子显微镜和计算方法阐明了钙钛矿表面出溶的多步机理。
In exsolution, nanoparticles form by emerging from oxide hosts by application of redox driving forces, leading to transformative advances in stability, activity, and efficiency over deposition techniques, and resulting in a wide range of new opportunities for catalytic, energy and net-zero-related technologies. However, the mechanism of exsolved nanoparticle nucleation and perovskite structural evolution, has, to date, remained unclear. Herein, we shed light on this elusive process by following in real time Ir nanoparticle emergence from a SrTiO3 host oxide lattice, using in situ high-resolution electron microscopy in combination with computational simulations and machine learning analytics. We show that nucleation occurs via atom clustering, in tandem with host evolution, revealing the participation of surface defects and host lattice restructuring in trapping Ir atoms to initiate nanoparticle formation and growth. These insights provide a theoretical platform and practical recommendations to further the development of highly functional and broadly applicable exsolvable materials. The separation of nanoparticles from oxide hosts by exsolution forms the basis for catalytic and energy-related applications. Here, the authors elucidate the multistep mechanism of exsolution at perovskite surfaces by combining real-time electron microscopy and computational methods.
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影响因子：
3.7
作者：
Kresse, G;Furthmuller, J
通讯作者：
Furthmuller, J
影响因子：
5.4
作者：
Bai, Lu;Li, Haibin;Li, Baoguang
通讯作者：
Li, Baoguang
影响因子：
0.6
作者：
Filimonov, S. N.;Hervieu, Yu Yu
通讯作者：
Hervieu, Yu Yu
DOI：
10.1016/0921-4534(94)90805-2
发表时间：
1994-08-01
影响因子：
1.7
作者：
NAITO, M;SATO, H
通讯作者：
SATO, H
影响因子：
16.6
作者：
Neagu D;Oh TS;Miller DN;Ménard H;Bukhari SM;Gamble SR;Gorte RJ;Vohs JM;Irvine JTS
通讯作者：
Irvine JTS