Modulating the Bader Charge Transfer in Single p-Block Atoms Doped Pd Metallene for Enhanced Oxygen Reduction Electrocatalysis
发布时间：2024-10-24
点击次数：
- 论文类型：
- Research Article
- 第一作者：
- Xie,Linfeng
- 通讯作者：
- Cai,Zhao,Li,Qing
- 合写作者：
- Huang,Yunhui,Yang,Feng,Cao,Ruiguo,Tanyuan,Lin,Zijie,Liang,Jiashun,Dr.,He,Zixu,Kun,Wang,Jing
- 发表刊物：
- Angewandte Chemie International Edition
- 所属单位：
- 华中科技大学
- 刊物所在地：
- 德国
- 文献类型：
- Article
- 卷号：
- 63
- 期号：
- 44
- 页面范围：
- e202407658
- ISSN号：
- 1521-3773
- 关键字：
- Pd metallene; p-d orbital hybridization; single-atom site; oxygen reduction reaction; Bader charge; zinc-air battery
- DOI码：
- 10.1002/anie.202407658
- 发表时间：
- 2024-07-29
- 影响因子：
- 16.1
- 摘要：
- Metallene is considered as an emerging family of electrocatalysts due to its atomically layered structure and unique surface stress. Here we propose a strategy to modulate the Bader charge transfer (BCT) between Pd surface and oxygenated intermediates via p-d electronic interaction by introducing single-atom p-block metal (M=In, Sn, Pb, Bi) into Pd metallene nanosheets towards efficient oxygen reduction reaction (ORR). X-ray absorption and photoelectron spectroscopy suggests that doping p-block metals could facilitate electron transfer to Pd sites and thus downshift the d-band center of Pd and weaken the adsorption energy of O intermediates. Among them, the developed Bi−Pd metallene shows extraordinarily high ORR mass activity of 11.34 A mgPd−1 and 0.86 A mgPd−1 at 0.9 V and 0.95 V in alkaline solution, respectively, representing the best Pd-based ORR electrocatalysts ever reported. In the cathode of a Zinc-air battery, Bi−Pd metallene could achieve an open-circuit voltage of 1.546 V and keep stable for 760 h at 10 mA cm−2. Theoretical calculations suggest that the BCT between Pd surface and *OO intermediates greatly affects the bond length between them (dPd-*OO) and Bi doping could appropriately reduce the amount of BCT and stretch the dPd-*OO, thus enhancing the ORR activity.
- 上一条：Tailoring Zirconia Supported Intermetallic Platinum Alloy via Reactive Metal-Support Interactions for High-Performing Fuel Cells
- 下一条：Single-atom Co dispersed on polyoxometalate derivatives confined in bamboo-like carbon nanotubes enabling efficient dual-site lattice oxygen mediated oxygen evolution electrocatalysis for acidic water electrolyzers