TY - JOUR

T1 - Scalable and Controllable Synthesis of Pt-Ni Bunched-Nanocages Aerogels as Efficient Electrocatalysts for Oxygen Reduction Reaction

AU - Zheng, Yuanyuan

AU - Petersen, Amanda Schramm

AU - Wan, Hao

AU - Hübner, René

AU - Zhang, Jiangwei

AU - Wang, Jianlan

AU - Qi, Haoyuan

AU - Ye, Yuhong

AU - Liang, Chaolun

AU - Yang, Jing

AU - Cui, Zhiming

AU - Meng, Yuezhong

AU - Zheng, Zhikun

AU - Rossmeisl, Jan

AU - Liu, Wei

N1 - Funding Information: Y.Z. and A.S.P. contributed equally to this work. Financial supports from the National Natural Science Foundation of China (52173296, 52061135103), the National Key Research and Development Program of China (2018YFA0702002), the Natural Science Foundation of Guangdong Province (2022A1515011826 and 2021A1515010650), the Science and Technology Projects of Guangzhou (202201011776 and 202102020918), the 100 Top Talents Program—Sun Yat‐sen University, and the open fund of Guangdong Key Laboratory of Fuel Cell Technology are gratefully acknowledged. Besides, the BL14W1 beamline of the Shanghai Synchrotron Radiation Facility (SSRF) and the 1W1B beamline of the Beijing Synchrotron Radiation Facility (BSRF) for providing beamtime are gratefully acknowledged. The Center for High Entropy Alloys Catalysis is sponsored by the Danish National Research Foundation Centers of Excellence, Project DNRF149. Additionally, A.S.P. and J.R. thank the Villum Foundation through the Villum Center for Science of Sustainable Fuels and Chemicals (No. 9455). The use of the HZDR Ion Beam Center TEM facilities and the funding of TEM Talos by the German Federal Ministry of Education and Research (BMBF; grant No. 03SF0451) in the framework of HEMCP are acknowledged. Publisher Copyright: © 2023 Wiley-VCH GmbH.

PY - 2023

Y1 - 2023

N2 - Developing efficient and stable Pt-based oxygen reduction reaction (ORR) electrocatalysts via both economical and controllable routes is critical for the practical application of electrochemical energy devices. Herein, a scalable, controllable, and general ambient-O2-involved aqueous-solution cultivating strategy to prepare PtxMy (M = Ni, Fe, Co) bunched-nanocages aerogels (BNCs AG) is demonstrated, based on a newly established high-M-to-Pt-precursor-ratio-and-B-incorporation-facilitated M-rich core and Pt-rich shell hydrogel formation process. The Pt83Ni17 BNCs AG shows prominent ORR performance with a mass activity (MA) of 1.95 A mgPt−1 and specific activity of 3.55 mA cm−2, which are 8.9-times and 9.6-times that of Pt supported on carbon (Pt/C), respectively. Particularly, the Pt83Ni17 BNCs AG displays greatly enhanced durability (MA 82.6% retention) compared to Pt/C (MA 31.8% retention) after a 20 000-cycles accelerated durability test. Systematic studies including density functional theory calculations uncover that the excellent activity is closely related to the optimized ligand and strain effects with the optimized Ni content in this aerogel; the outstanding durability is endowed by the lowered-down Ni leaching with the optimized Pt/Ni ratio and the inhibited sintering due to its appropriate porosity. This work provides new perspectives on the development of electrocatalysts with both high performance and low cost.

AB - Developing efficient and stable Pt-based oxygen reduction reaction (ORR) electrocatalysts via both economical and controllable routes is critical for the practical application of electrochemical energy devices. Herein, a scalable, controllable, and general ambient-O2-involved aqueous-solution cultivating strategy to prepare PtxMy (M = Ni, Fe, Co) bunched-nanocages aerogels (BNCs AG) is demonstrated, based on a newly established high-M-to-Pt-precursor-ratio-and-B-incorporation-facilitated M-rich core and Pt-rich shell hydrogel formation process. The Pt83Ni17 BNCs AG shows prominent ORR performance with a mass activity (MA) of 1.95 A mgPt−1 and specific activity of 3.55 mA cm−2, which are 8.9-times and 9.6-times that of Pt supported on carbon (Pt/C), respectively. Particularly, the Pt83Ni17 BNCs AG displays greatly enhanced durability (MA 82.6% retention) compared to Pt/C (MA 31.8% retention) after a 20 000-cycles accelerated durability test. Systematic studies including density functional theory calculations uncover that the excellent activity is closely related to the optimized ligand and strain effects with the optimized Ni content in this aerogel; the outstanding durability is endowed by the lowered-down Ni leaching with the optimized Pt/Ni ratio and the inhibited sintering due to its appropriate porosity. This work provides new perspectives on the development of electrocatalysts with both high performance and low cost.

KW - aerogels

KW - electrocatalysts

KW - fuel cells

KW - nanocages

KW - oxygen reduction reaction

U2 - 10.1002/aenm.202204257

DO - 10.1002/aenm.202204257

M3 - Journal article

AN - SCOPUS:85150713949

VL - 13

JO - Advanced Energy Materials

JF - Advanced Energy Materials

SN - 1614-6832

IS - 20

M1 - 2204257

ER -