High-throughput, combinatorial synthesis of multimetallic nanoclusters
High-throughput, combinatorial synthesis of multimetallic nanoclusters
复制标题
DOI：
10.1073/pnas.1903721117
复制
发表时间：
2020-03
影响因子：
11.1
通讯作者：
Yonggang Yao;Zhennan Huang;Tangyuan Li;Hang Wang;Yifan Liu;H. Stein;Y. Mao;Jinlong Gao;Miao-lun Jiao;Qi Dong;J. Dai;Pengfei Xie;Hua Xie;Steven D. Lacey;I. Takeuchi;J. Gregoire;R. Jiang;Chao Wang;André D. Taylor;R. Shahbazian‐Yassar;Liangbing Hu
中科院分区：
文献类型：
--
作者：
Yonggang Yao;Zhennan Huang;Tangyuan Li;Hang Wang;Yifan Liu;H. Stein;Y. Mao;Jinlong Gao;Miao-lun Jiao;Qi Dong;J. Dai;Pengfei Xie;Hua Xie;Steven D. Lacey;I. Takeuchi;J. Gregoire;R. Jiang;Chao Wang;André D. Taylor;R. Shahbazian‐Yassar;Liangbing Hu
意义多元素纳米材料由于其广泛可调的表面化学而具有广泛的应用前景，但有效地研究这个多维空间仍然是一个挑战。传统的方法通常是缓慢的，依赖于机缘巧合，而在日益复杂的构图中，仍然缺乏健壮和普遍的合成。我们报道了一种高通量技术，用于组合组成设计(溶液相配方)和快速合成(在几秒钟内)具有均匀合金结构的超细多金属纳米团簇。我们用液滴电池扫描电化学法合成和筛选了PtPdRhRuIrFeCoNi组成空间，两种有希望的催化剂迅速被鉴定出来，并在转盘装置上得到进一步验证。报道的高通量方法建立了一条简单可靠的管道，大大加快了多金属纳米材料的材料发现。多金属纳米团簇(MMNC)提供了独特的、可定制的表面化学，具有巨大的催化应用潜力。为了有效地探索这一广阔的化学空间，需要一条加速发现管道，以取代传统的“试错”实验，同时确保统一的微结构，尽管成分复杂。在这里，我们报道了一系列广泛的超细且均匀的合金MMNC的高通量合成，通过1)在前驱体溶液相中通过配方进行灵活的成分设计和2)利用热冲击加热(即∼1,650K，∼500ms)超快合成合金MMNC。与传统的气相沉积相比，这种方法非常简单和容易获得，并且颗粒大小和结构均匀度使得能够对成分不同的MMNC进行比较研究。使用扫描液滴池演示了快速电化学筛选，使我们能够发现两个有希望的电催化剂，我们随后使用旋转圆盘装置进行了验证。这一展示的高通量材料发现管道为方便和加速探索广泛应用的跨国公司提供了一个范例。
Significance Multielement nanomaterials hold great promise for various applications due to their widely tunable surface chemistry, yet it remains challenging to efficiently study this multidimensional space. Conventional approaches are typically slow and depend on serendipity, while a robust and general synthesis is still lacking among increasingly complex compositions. We report a high-throughput technique for combinatorial compositional design (formulation in solution phases) and rapid synthesis (within seconds) of ultrafine multimetallic nanoclusters with a homogeneous alloy structure. We synthesized and screened the PtPdRhRuIrFeCoNi compositional space using scanning droplet cell electrochemistry, with two promising catalysts quickly identified and further verified in a rotating disk setup. The reported high-throughput approach establishes a facile and reliable pipeline to significantly accelerate material discovery in multimetallic nanomaterials. Multimetallic nanoclusters (MMNCs) offer unique and tailorable surface chemistries that hold great potential for numerous catalytic applications. The efficient exploration of this vast chemical space necessitates an accelerated discovery pipeline that supersedes traditional “trial-and-error” experimentation while guaranteeing uniform microstructures despite compositional complexity. Herein, we report the high-throughput synthesis of an extensive series of ultrafine and homogeneous alloy MMNCs, achieved by 1) a flexible compositional design by formulation in the precursor solution phase and 2) the ultrafast synthesis of alloy MMNCs using thermal shock heating (i.e., ∼1,650 K, ∼500 ms). This approach is remarkably facile and easily accessible compared to conventional vapor-phase deposition, and the particle size and structural uniformity enable comparative studies across compositionally different MMNCs. Rapid electrochemical screening is demonstrated by using a scanning droplet cell, enabling us to discover two promising electrocatalysts, which we subsequently validated using a rotating disk setup. This demonstrated high-throughput material discovery pipeline presents a paradigm for facile and accelerated exploration of MMNCs for a broad range of applications.