Low temperature synthesis of new highly graphitized N-doped carbon for Pt fuel cell supports, satisfying DOE 2025 durability standards for both catalyst and support

被引:39
作者
Lee, Ha-Young [1 ]
Yu, Ted H. [2 ]
Shin, Cheol-Hwan [1 ]
Fortunelli, Alessandro [2 ,3 ]
Ji, Sang Gu [4 ]
Kim, Yujin [5 ]
Kang, Tong-Hyun [1 ]
Lee, Byong-June [1 ]
Merinov, Boris V. [2 ]
Goddard, William A., III [2 ]
Choi, Chang Hyuck [5 ]
Yu, Jong-Sung [1 ,6 ]
机构
[1] Daegu Gyeongbuk Inst Sci & Technol DGIST, Dept Energy Sci & Engn, Daegu 42988, South Korea
[2] CALTECH, Mat & Proc Simulat Ctr, Pasadena, CA 91125 USA
[3] CNR, CNR ICCOM, I-56124 Pisa, Italy
[4] Gwangju Inst Sci & Technol GIST, Sch Mat Sci & Engn, Gwangju 61005, South Korea
[5] Pohang Univ Sci & Technol POSTECH, Dept Chem, Pohang 37673, South Korea
[6] DGIST, Energy Sci & Engn Res Ctr, Daegu 42988, South Korea
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2023年 / 323卷
关键词
PEMFCs; Graphitized carbon; Pyrrolic-N; Real-time degradation analysis; Grand canonical reaction kinetics; NITROGEN; ELECTROCATALYSTS; PERFORMANCE; NITRIDE; DEGRADATION; OPERATION; GRAPHENE;
D O I
10.1016/j.apcatb.2022.122179
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
For polymer electrolyte membrane fuel cells (PEMFCs), the state-of-the-art electrocatalysts are based on carbon -supported Pt group metals. However, current carbon supports suffer from carbon corrosion during repeated start -stop operations, causing performance degradation. We report a new strategy to produce highly graphitized carbon with controllable N-doping that uses low-temperature synthesis (650 celcius) from g-C3N4 carbon-nitrogen precursor with pyrolysis using Mg. The high graphiticity is confirmed by high-intensity 2D Raman peak with low ID/IG (0.57), pronounced graphitic XRD planes, and excellent conductivity. Without further post-treatment, this highly graphitized N-doped carbon (HGNC) material combines high pyrrolic-N content with high porosity. Supporting Pt on HGNC exhibits excellent oxygen reduction activity for PEMFC with greatly improved durability as proved by real-time loss measurements of Pt and carbon, the first to surpass the DOE 2025 durability targets for both catalyst and support. The Pt/HGNC-65 shows 32% and 24% drop in mass activity after accelerated durability tests of both electrocatalyst and support, respectively, which are less than DOE target of 40% loss. The atomistic basis for this durability is explained via quantum mechanics-based molecular dynamics simulations. Interestingly, it is found that pyrrolic-N strongly interacts with Pt, making the Pt catalyst more stable during fuel cell reaction.
引用
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页数:11
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