期刊
ACS NANO
卷 14, 期 10, 页码 13279-13293出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c05088
关键词
single atom catalyst; graphene; phthalocyanine; water oxidation; oxygen reduction; operando X-ray absorption spectroscopy
类别
资金
- University of Zurich Research Priority Program (URPP) for Solar Light to Chemical Energy Conversion (LightChEC)
- Swiss National Science Foundation [CRSII2_160801]
- China Scholarship Council (CSC)
- Diamond Light Source [EM16967]
- Swiss National Science Foundation (SNF) [CRSII2_160801] Funding Source: Swiss National Science Foundation (SNF)
Y Single atom catalysts (SACs) are ideal model systems in catalysis research. Here we employ SACs to address the fundamental catalytic challenge of generating well-defined active metal centers to elucidate their interactions with coordinating atoms, which define their catalytic performance. We introduce a soft-landing molecular strategy for tailored SACs based on metal phthalocyanines (MPcs, M = Ni, Co, Fe) on graphene oxide (GO) layers to generate well-defined model targets for mechanistic studies. The formation of electronic channels through pi-pi conjugation with the graphene sheets enhances the MPc-GO performance in both oxygen evolution and reduction reactions (OER and ORR). Density functional theory (DFT) calculations unravel that the outstanding ORR activity of FePc-GO among the series is due to the high affinity of Fe atoms toward O-2 species. Operando X-ray absorption spectroscopy and DFT studies demonstrate that the OER performance of the catalysts relates to thermodynamic or kinetic control at low- or high-potential ranges, respectively. We furthermore provide evidence that the participation of ligating N and C atoms around the metal centers provides a wider selection of active OER sites for both NiPc-GO and CoPc-GO. Our strategy promotes the understanding of coordination-activity relationships of high-performance SACs and their optimization for different processes through tailored combinations of metal centers and suitable ligand environments.
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