Liang Ding
(, ), Ze-Cheng Yao
(, ), Tang Tang
(, ), Xin Wan
(, ), Xiaozhi Liu
(, ), Zhe Jiang
(, ), Jiaju Fu
(, ), Zhuo-Qi Shi
(, ), Jing Tai
(, ), Zhen-Hua Lyu
(, ), Jichen Dong
(, ), Qing Li
(, ), Dong Su
(, ), Jianglan Shui
(, ), Jin-Song Hu
(, ), Li-Jun Wan
(, )
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引用次数: 0
Abstract
High-performance cathode catalysts are essential for proton-exchange membrane fuel cells. Intermetallic nanocrystals are promising candidates but suffer from intrinsic activity–durability trade-offs because their comprehensive catalytic properties are determined by several intertwined structural factors that cannot be optimized independently by existing synthesis techniques. The challenge lies in the inherent thermodynamic and kinetic constraints during synthesis. Here we develop a decoupled synthesis strategy that leverages block-copolymer micelle confinement, which enables the customized synthesis of libraries of intermetallic nanocrystals, simultaneously achieving ultra-small size, ultra-high ordering degree, tailorable loading density, narrow size distribution, compositional uniformity, and broad compositional and substrate universality. The developed Pt3Co intermetallic nanocrystal/Ketjenblack catalyst achieves a rated power density of 1.08 W cm−2 and 92% rated power retention after 30,000 cycles under light-duty-vehicle conditions and 900 h of stable operation at 10 A. It also delivered a 70.2% cell efficiency without degradation and 98.4% specific power retention after 90,000 cycles of heavy-duty-vehicle applications. This performance led us to project a lifetime of 240,000 h. Oxygen reduction catalysts are critical for advancing the durability and efficiency of proton-exchange membrane fuel cells (PEMFCs). Now a block-copolymer micelle confinement strategy is shown to enable the decoupled synthesis of highly ordered, ultra-dense Pt-based intermetallic nanocrystals, yielding PEMFC catalysts with high activity and long projected lifetimes.
高性能阴极催化剂是质子交换膜燃料电池的重要组成部分。金属间纳米晶体是很有前途的候选材料,但由于其综合催化性能是由几个相互交织的结构因素决定的,而这些因素无法通过现有的合成技术独立优化。挑战在于合成过程中固有的热力学和动力学约束。在这里,我们开发了一种解耦合成策略,利用嵌段共聚物胶束约束,使金属间纳米晶体库的定制合成成为可能,同时实现了超小尺寸、超高有序度、可定制的负载密度、窄尺寸分布、成分均匀性以及广泛的成分和衬底通用性。开发的Pt3Co金属间纳米晶/Ketjenblack催化剂在轻型车辆条件下循环30,000次,在10 a下稳定运行900小时后,额定功率密度为1.08 W cm−2,额定功率保持率为92%。在重型车辆应用90000次循环后,它还提供了70.2%的电池效率和98.4%的比功率保持率。这一性能使我们预计寿命为24万小时。
期刊介绍:
Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry.
Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.