Journal ArticleDOI
Atomically dispersed single iron sites for promoting Pt and Pt3Co fuel cell catalysts: performance and durability improvements
Zhi Qiao,Chenyu Wang,Chenzhao Li,Yachao Zeng,Sooyeon Hwang,Boyang Li,Stavros Karakalos,Jaehyung Park,A. Jeremy Kropf,Evan C. Wegener,Qing Gong,Hui Xu,Guofeng Wang,Deborah J. Myers,Jian Xie,Jacob S. Spendelow,Gang Wu +16 more
TLDR
In this paper, an effective strategy to boost PGM catalysts through integrating PGM-free atomically-dispersed single metal active sites in the carbon support toward the cathode oxygen reduction reaction (ORR) was reported.Abstract:
Significantly reducing platinum group metal (PGM) loading while improving catalytic performance and durability is critical to accelerating proton-exchange membrane fuel cells (PEMFCs) for transportation. Here we report an effective strategy to boost PGM catalysts through integrating PGM-free atomically-dispersed single metal active sites in the carbon support toward the cathode oxygen reduction reaction (ORR). We achieved uniform and fine Pt nanoparticle (NP) (∼2 nm) dispersion on an already highly ORR-active FeN4 site-rich carbon (FeN4–C). Furthermore, we developed an effective approach to preparing a well-dispersed and highly ordered L12 Pt3Co intermetallic nanoparticle catalyst on the FeN4–C support. DFT calculations predicted a synergistic interaction between Pt clusters and surrounding FeN4 sites through weakening O2 adsorption by 0.15 eV on Pt sites and reducing activation energy to break O–O bonds, thereby enhancing the intrinsic activity of Pt. Experimentally, we verified the synergistic effect between Pt or Pt3Co NPs and FeN4 sites, leading to significantly enhanced ORR activity and stability. Especially in a membrane electrode assembly (MEA) with a low cathode Pt loading (0.1 mgPt cm−2), the Pt/FeN4–C catalyst achieved a mass activity of 0.451 A mgPt−1 and retained 80% of the initial values after 30 000 voltage cycles (0.60 to 0.95 V), exceeding DOE 2020 targets. Furthermore, the Pt3Co/FeN4 catalyst achieved significantly enhanced performance and durability concerning initial mass activity (0.72 A mgPt−1), power density (824 mW cm−2 at 0.67 V), and stability (23 mV loss at 1.0 A cm−2). The approach to exploring the synergy between PGM and PGM-free Fe–N–C catalysts provides a new direction to design advanced catalysts for hydrogen fuel cells and various electrocatalysis processes.read more
Citations
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Journal ArticleDOI
Atomically dispersed Pt and Fe sites and Pt–Fe nanoparticles for durable proton exchange membrane fuel cells
Fei Xiao,Qi Wang,Gui-Liang Xu,Xueping Qin,Inhui Hwang,Cheng-Jun Sun,Min Liu,Wei Hua,Hsi-wen Wu,Shangqian Zhu,Jin-Cheng Li,Jian-Gan Wang,Yuanmin Zhu,Duojie Wu,Zidong Wei,Meng Gu,Khalil Amine,Minhua Shao +17 more
TL;DR: In this article , a hybrid electrocatalyst that consists of atomically dispersed Pt and Fe single atoms and Pt-Fe alloy nanoparticles was designed. But the performance of the hybrid was limited by the high cost and low durability of Pt-based electrocatalysts.
Journal ArticleDOI
Mutual-modification Effect in Adjacent Pt Nanoparticles and Single Atoms with Sub-nanometer Inter-site Distances to Boost Photocatalytic Hydrogen Evolution
Manyi Gao,Fenyang Tian,Zhi-Bing Guo,Xin Zhang,Zhijun Li,Jing Zhou,Xin-jing Zhou,Yongsheng Yu,Weiwei Yang +8 more
TL;DR: In this article , an atom-like Pt@PtSAs co-catalyst on polymeric carbon nitride nanosheets (PCNS), where the mutual modification effect exists in nucleuslike Pt NPs and diffuse PtSAs with sub-nanometer inter-site distances, was reported.
Journal ArticleDOI
PGM-Free Oxygen-Reduction Catalyst Development for Proton-Exchange Membrane Fuel Cells: Challenges, Solutions, and Promises
Yanghua He,Gang Wu +1 more
TL;DR: In this article , the authors highlight recent advances in synthesizing efficient PGM-free catalysts for the ORR in PEMFCs, emphasizing effective strategies to improve mass and intrinsic activity and the possible degradation mechanisms.
Journal ArticleDOI
Tuning Two‐Electron Oxygen‐Reduction Pathways for H2O2 Electrosynthesis via Engineering Atomically Dispersed Single Metal Site Catalysts
TL;DR: In this article , a structure-property correlation is used to guide rational catalysts design with a favorable 2e−ORR process. But, the performance metrics and knowledge during the electrolyzer development are highlighted.
Journal ArticleDOI
Atomic Structure Evolution of Pt-Co Binary Catalysts: Single Metal Sites versus Intermetallic Nanocrystals.
Xing Li,Xing Li,Xing Li,Yanghua He,Shaobo Cheng,Boyang Li,Yachao Zeng,Zhenhua Xie,Qingping Meng,Lu Ma,Kim Kisslinger,Xiao Tong,Sooyeon Hwang,Siyu Yao,Chenzhao Li,Zhi Qiao,Chongxin Shan,Yimei Zhu,Jian Xie,Guofeng Wang,Gang Wu,Dong Su,Dong Su +22 more
TL;DR: In this article, the thermally driven structure evolution of Pt-Co binary catalysts is investigated using advanced in situ electron microscopy, including PtCo intermetallic alloys and single Pt/Co metal sites.
References
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ATHENA, ARTEMIS, HEPHAESTUS: data analysis for X-ray absorption spectroscopy using IFEFFIT.
Bruce Ravel,Matthew Newville +1 more
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High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
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Journal Article
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
TL;DR: In this article, a family of non-precious metal catalysts that approach the performance of platinum-based systems at a cost sustainable for high-power fuel cell applications, possibly including automotive power.
Journal ArticleDOI
Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
Jeffrey Greeley,Ifan E. L. Stephens,Alexander S. Bondarenko,Tobias Peter Johansson,Heine Anton Hansen,Thomas F. Jaramillo,Thomas F. Jaramillo,Jan Rossmeisl,Ib Chorkendorff,Jens K. Nørskov +9 more
TL;DR: A new set of ORR electrocatalysts consisting of Pd or Pt alloyed with early transition metals such as Sc or Y, identified using density functional theory calculations as being the most stable Pt- and Pd-based binary alloys with ORR activity likely to be better than Pt.
Journal ArticleDOI
Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces
Chen Chen,Yijin Kang,Ziyang Huo,Ziyang Huo,Zhongwei Zhu,Zhongwei Zhu,Wenyu Huang,Wenyu Huang,Huolin L. Xin,Joshua Snyder,Dongguo Li,Jeffrey A. Herron,Manos Mavrikakis,Miaofang Chi,Karren L. More,Yadong Li,Nenad M. Markovic,Gabor A. Somorjai,Gabor A. Somorjai,Peidong Yang,Vojislav R. Stamenkovic +20 more
TL;DR: A highly active and durable class of electrocatalysts is synthesized by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals by exploitingThe starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility.
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