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吉宗 航*; Kikkawa, Nobuaki*; Yoneyama, Hiroaki*; Takahashi, Naoko*; Minami, Saori*; Akimoto, Yusuke*; Mitsuoka, Takuya*; Kawaura, Hiroyuki*; Harada, Masashi*; 山田 悟史*; et al.
ACS Applied Materials & Interfaces, 14(48), p.53744 - 53754, 2022/11
被引用回数:7 パーセンタイル:63.54(Nanoscience & Nanotechnology)Chemically modified carbon supports for the cathode catalyst layers of polymer electrolyte fuel cells (PEFCs) show considerable promise for boosting the oxygen reduction reaction. This study evaluated the ionomer distribution of Nafion ionomer thin films on nitrogen (N)-modified carbon surfaces along their depth direction. Neutron reflectivity (NR) measurements performed using the double-contrast technique with HO and DO revealed that the introduction of N functional groups to carbon thin films promoted ionomer adsorption onto the surface under wet conditions (22C, 85% relative humidity). Molecular dynamics (MD) simulations conducted to verify the origin of the robust contact between the ionomer and N-modified carbon surface revealed an ionomer adsorption mechanism on the N-modified carbon surfaces, which involved Coulomb interactions between the positively charged carbon surface and the ionomer side chains with negatively charged sulfonic acid groups. The positive surface charge, which was determined using the contents of the N functional groups estimated by X-ray photoelectron spectroscopy, was found to be sufficient as an impetus for ionomer adsorption. This strategy involving NR measurements and MD simulations can provide insights into the solid-ionomer interfacial structures in a cathode catalyst layer and can therefore be extensively employed in studies on PEFCs.
引間 和浩*; 日沼 洋陽*; 清水 啓佑*; 鈴木 耕太*; 田港 聡*; 平山 雅章*; 増田 卓也*; 田村 和久; 菅野 了次*
ACS Applied Materials & Interfaces, 13(6), p.7650 - 7663, 2021/02
被引用回数:12 パーセンタイル:66.55(Nanoscience & Nanotechnology)(001)配向したLiMnO薄膜を正極とした全固体リチウムイオン電池を作成し、表面X線回折法で表面構造を解析した。LiPOをコーティングした電極は、徐々に活性化し、活性化が終わると電池容量は維持されることがわかった。LiPOをコーティングした正極では、表面におけるMnやOの組成の変化がないためであると結論した。すなわち、本系は充放電に対して安定である特長を有することが判明した。このことはまた、今後の実用化に向け、重要な知見を与える結果である。
Zheng, Y.*; Xiao, H.*; Li, K.*; Wang, Y.*; Li, Y.*; Wei, Y.*; Zhu, X.*; Li, H.-W.*; 松村 大樹; Guo, B.*; et al.
ACS Applied Materials & Interfaces, 12(37), p.42274 - 42284, 2020/09
被引用回数:22 パーセンタイル:74.29(Nanoscience & Nanotechnology)Interactions between the active components with the support are one of the fundamentally factors in determining the catalytic performance of a catalyst. In this study, we investigated the interaction between CeO and LaFeO, the two important oxygen storage materials in catalysis area, by tuning the sizes of CeO particles and highlight a two-fold effect of the strong oxide-oxide interaction in determining the catalytic activity and selectivity for preferential CO oxidation in hydrogen feeds. It is found that the anchoring of ultra-fine CeO particles at the framework of three-dimensional-ordered macroporous LaFeO surface results in a strong interaction between the two oxides that induces the formation of abundant uncoordinated cations and oxygen vacancy at the interface. This discovery demonstrates that in hybrid oxide-based catalysts, tuning the interaction among different components is essential for balancing the catalytic activity and selectivity.
Zhang, Z,*; Wang, H.*; 吉川 浩史*; 松村 大樹; 畑尾 秀哉*; 石川 理史*; 上田 渉*
ACS Applied Materials & Interfaces, 12(5), p.6056 - 6063, 2020/02
被引用回数:6 パーセンタイル:30.33(Nanoscience & Nanotechnology)Developing new cathode-active materials for rechargeable batteries is important to fulfill the growing demands of energy transformation, storage, and utilization. Zeolitic transition-metal oxides based on vanadomolybdate, constructed by pentagon metal-oxygen clusters as building blocks and metal ions as linkers in a trigonal symmetry, are good candidates for cathodes of Na rechargeable batteries. The material is activated via amorphization of the crystal structure in the ab plane during discharging process, keeping the molecular structure of the building blocks stable, which causes high specific capacity and good cycle performance.
府金 慶介*; 森 利之*; Yan, P.*; 増田 卓也*; 山本 春也; Ye, F.*; 吉川 英樹*; Auchterlonie, G.*; Drennan, J.*
ACS Applied Materials & Interfaces, 7(4), p.2698 - 2707, 2015/02
被引用回数:30 パーセンタイル:66.8(Nanoscience & Nanotechnology)白金-酸化セリウム(Pt-CeO(1.52))は、Ptカソードよりも高い酸素還元反応活性を示すことから、固体高分子形燃料電池のカソード極に使用する電極材料として有望視されている。本研究では、Pt-CeOの高い酸素還元活性の発現に関係しているとして考えられているPt-CeOヘテロ界面の微細構造を明らかにすることを目的に、パルスレーザー蒸着法により導電性を有するNb:SrTiO単結晶基板上にCeOのエピタキシャル膜を形成し、さらにCeO膜上に含浸法によりPt粒子を形成してPtとCeO界面構造が単純化されたPt-CeO薄膜カソードを作製した。透過型電子顕微鏡によるPt-CeO界面の構造評価及び電気化学測定による酸素還元反応活性評価、さらに格子動力学計算結果との比較により界面構造を調べた結果、Pt-CeO界面に形成されるPt-O-酸素欠陥-セリウム欠陥構造が高い酸素還元活性の発現に関係していることが示唆された。
Ma, H.*; Chi, H.*; Wu, J.*; Wang, M.*; Li, J.*; 保科 宏行; 佐伯 誠一; 瀬古 典明
ACS Applied Materials & Interfaces, 5(17), p.8761 - 8765, 2013/09
被引用回数:14 パーセンタイル:42.85(Nanoscience & Nanotechnology)Gold nanostructured microtubes (AuNMTs) are prepared using a tertiary amine group-functionalized polyethylene (PE)-coated polypropylene (PP) nonwoven fabric as a ligand, a reductant, and a template, which takes advantage of the different radiation effects of PE and PP. The Au(III) ions are absorbed and reduced only in the PE layer to form the aggregation of gold nanoparticles; thus, AuNMTs are obtained after the calcination.