Configuration-Dependent Oxygen Reduction Reaction Performance of Iridium-Decorated Ni@Pd Nanocatalysts

被引：6

作者：

Bhalothia, Dinesh ^{[1
]}

Wang, Sheng-Po ^{[2
]}

Chen, Pei-You ^{[2
]}

Wu, Han-Po ^{[2
]}

Beniwal, Amisha ^{[1
]}

Yan, Che ^{[1
]}

Lee, Jyh-Fu ^{[3
]}

Chen, Tsan-Yao ^{[1
,4
]}

Chen, Po-Chun ^{[2
]}

机构：

[1] Natl Tsing Hua Univ, Dept Engn & Syst Sci, Hsinchu 30013, Taiwan

[2] Natl Taipei Univ Technol, Dept Mat & Mineral Resources Engn, Taipei 10608, Taiwan

[3] Natl Synchrotron Radiat Res Ctr NSRRC, Hsinchu 30076, Taiwan

[4] Natl Cheng Kung Univ, Hierarch Green Energy Mat Hi GEM Res Ctr, Tainan 70101, Taiwan

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2023年 / 127卷 / 20期

关键词：

ORR ACTIVITY; CATALYSTS;

D O I：

10.1021/acs.jpcc.3c01468

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：

The widespread market introduction of fuel cells is severelyrestrictedby the sluggish oxygen reduction reaction (ORR) kinetics at the cathodeside, which demands highly efficient and durable catalysts for generatingadequate rates. By keeping this in view, herein, we report a systematicstudy to unveil the effect of structure configuration on the ORR activityof tri-metallic nanocatalysts (NC)-s comprising atomic iridium (Ir)cluster (0.5 wt % of Ir)-anchored Pd nanoparticles (NP)-s on the tetrahedralsymmetric Ni-oxide support (denoted as NPI), prepared via a temperature-controlledwet chemical reduction method. For the optimum condition when theimpregnation temperature for Ni-crystal growth is 40 degrees C, theIr-cluster-decorated Ni@Pd nanoislands are formed (hereafter denotedas NPI-40), outperforming the commercial Johnson Matthey-Pt/C (J.M.-Pt/C;20 wt % Pt) catalyst by 181-fold with an unprecedented high mass activityof 12,163 mAmg(Ir) (-1) at 0.85 V vs RHE inalkaline ORR (0.1 M KOH). More importantly, NPI-40 NC retained 100%ORR performance with no degradation up to 20,000 accelerated degradationtest (ADT) cycles, while only a 5 mV loss in half-wave potential (E (1/2)) is observed after 30 k ADT cycles. Besides,Ir-cluster-decorated Ni-core@unconformable Pd-shell and Ni-to-Pd epitaxial structures are formed at 25 degrees C (NPI-RT)and 70 degrees C (NPI-70) impregnation temperatures, respectively, showingthe significantly decreased mass activities of 997 and 5146 mAmg(Ir) (-1) at 0.85 V vs RHE. The results of physicalstructure inspections and electrochemical analysis suggest that suchan exceptional ORR performance of NPI-40 NC originates from the potentialsynergism between the high density of the occupied Ir-d orbital andthe adjacent compressively strained Ni-Pd interface, whereIr sites offer optimal adsorption energy for O-2 splittingand the Ni-Pd interface facilitates the subsequent desorptionof hydroxide ions (OH-). We believe that the obtainedresults will open new avenues for the facile design of Pt-free NCsfor fuel cell cathodes and will benefit fuel-cell technology via bothecologically and economically friendly means.

引用

页码：9594 / 9602

页数：9

共 34 条

[1] NiOx-supported PtRh nanoalloy enables high-performance hydrogen evolution reaction under universal pH conditions [J].