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論文

Structure of active sites of Fe-N-C nano-catalysts for alkaline exchange membrane fuel cells

岸 浩史*; 坂本 友和*; 朝澤 浩一郎*; 山口 進*; 加藤 豪士*; Zulevi, B.*; Serov, A.*; Artyushkova, K.*; Atanassov, P.*; 松村 大樹; et al.

Nanomaterials (Internet), 8(12), p.965_1 - 965_13, 2018/12

 被引用回数:10 パーセンタイル:49.61(Chemistry, Multidisciplinary)

Platinum group metal-free catalysts based on transition metal-nitrogen-carbon nanomaterials have been studied by a combination of in situ X-ray spectroscopy techniques, high-resolution transmission electron microscope, M$"o$ssbauer spectroscopy, electrochemical methods and density functional theory. Fe-N-C oxygen reduction reaction electrocatalysts were synthesized by varying several synthetic parameters to obtain nanomaterials with different composition and morphology. Associated with Fe-N$$_x$$ motive and the presence of Fe metallic particles in the electrocatalysts showed the clear differences in the variation of composition; processing and treatment conditions of sacrificial support method. From the results of material characterization; catalytic activity and theoretical studies; Fe metallic particles (coated with carbon) are main contributors into the HO$$_{2}$$$$^{-}$$ generation.

論文

Study of catalytic reaction at electrode-electrolyte interfaces by a CV-XAFS method

草野 翔吾*; 松村 大樹; 朝澤 浩一郎*; 岸 浩史*; 坂本 友和*; 山口 進*; 田中 裕久*; 水木 純一郎*

Journal of Electronic Materials, 46(6), p.3634 - 3638, 2017/06

 被引用回数:3 パーセンタイル:19.95(Engineering, Electrical & Electronic)

A method combining cyclic voltammetry (CV) with X-ray absorption fine structure (XAFS) spectroscopy, viz. CV-XAFS, has been developed to enable in situ real-time investigation of atomic and electronic structures related to electrochemical reactions. We use this method to study the reaction of a Pt/C cathode catalyst in the oxygen reduction reaction (ORR) in an alkaline electrolyte. It was found that the current induced by the ORR was first observed at approximately 0.08 V versus Hg/HgO, although the Pt valence remained almost unchanged. The electronic structure of the catalytic surface in the ORR was observed to be different in the negative and positive scan directions of CV measurements. Hydrogen adsorption is also discussed on the basis of the observation of this spectral change. We have demonstrated that CV-XAFS provides dynamical structural and electronic information related to electrochemical reactions and can be used for in situ real-time measurements of a catalyst.

論文

NiO/Nb$$_{2}$$O$$_{5}$$/C hydrazine electrooxidation catalysts for anion exchange membrane fuel cells

坂本 友和*; 増田 晃之*; 吉本 光児*; 岸 浩史*; 山口 進*; 松村 大樹; 田村 和久; 堀 彰宏*; 堀内 洋輔*; Serov, A.*; et al.

Journal of the Electrochemical Society, 164(4), p.F229 - F234, 2017/01

 被引用回数:12 パーセンタイル:40.97(Electrochemistry)

NiO/ Nb$$_{2}$$O$$_{5}$$/C (8:1), (4:1), (2:1), NiO/C, and Ni/C catalysts for hydrazine electrooxidation were synthesized by an evaporation drying method followed by thermal annealing. Prepared catalysts were characterized by X-ray diffraction (XRD), high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), energy dispersive X-ray spectrometry (EDS), and X-ray absorption fine structure (XAFS). The highest catalytic activity in mentioned above reactionwas found for Ni/C, followed by: NiO/Nb$$_{2}$$O$$_{5}$$/C (8:1), NiO/Nb$$_{2}$$O$$_{5}$$/C (4:1). NiO/Nb$$_{2}$$O$$_{5}$$/C (2:1) whiles NiO/C has almost no activity for hydrazine oxidation. It was explained by oxygen defect of NiO in NiO/ Nb$$_{2}$$O$$_{5}$$/C from XAFS analysis. The selectivity hydrazine electrooxidation as measured by ammonia production resulted in observation that metallic Ni surface facilitates N-N bond breaking of hydrazine, which was confirmed by density functional theory (DFT) calculations.

論文

Mechanism study of hydrazine electrooxidation reaction on nickel oxide surface in alkaline electrolyte by in situ XAFS

坂本 友和*; 岸 浩史*; 山口 進*; 松村 大樹; 田村 和久; 堀 彰宏*; 堀内 洋輔*; Serov, A.*; Artyushkova, K.*; Atanassov, P.*; et al.

Journal of the Electrochemical Society, 163(10), p.H951 - H957, 2016/08

 被引用回数:28 パーセンタイル:76.71(Electrochemistry)

The catalytic process takes place on nickel oxide surface of a Ni oxide nano-particle decorated carbon support (NiO/C). In-situ X-ray absorption fine structure (XAFS) spectroscopy was used to investigate the reaction mechanism for hydrazine electrooxidation on NiO surface. The spectra of X-ray absorption near-edge structure (XANES) of Ni K-edge indicated that adsorption of OH$$^{-}$$ on Ni site during the hydrazine electrooxidation reaction. Density functional theory (DFT) calculations were used to elucidate and suggest the mechanism of the electrooxidation and specifically propose the localization of electron density from OH$$^{-}$$ to 3d orbital of Ni in NiO. It is found that the accessibility of Ni atomic sites in NiO structure is critical for hydrazine electrooxidation. Based on this study, we propose a possible reaction mechanism for selective hydrazine electrooxidation to water and nitrogen taking place on NiO surface as it is applicable to direct hydrazine alkaline membrane fuel cells.

論文

アニオン形燃料電池用非白金系電極触媒の開発

坂本 友和*; 岸 浩史*; 山口 進*; 田中 裕久*; 松村 大樹; 田村 和久; 西畑 保雄

表面科学, 37(2), p.78 - 83, 2016/02

自動車のゼロエミッション化は、環境対策技術における重要な取り組みの1つであり、そのうえで燃料電池車の開発は重要となっている。燃料電池車が普及する上で重要なのは、燃料コストが低く、インフラ整備が容易であることであり、これを満たすのは、電池材料が非貴金属で構成可能であり燃料が液体である、ヒドラジンを燃料とするアニオン形燃料電池である。我々はこのヒドラジンを燃料とするアニオン形燃料電池を開発しており、すでに2013年に試作車が完成する段階まで進んでいる。本稿では、燃料電池の心臓部である、電極触媒の開発について解説する。

論文

Towards optimizing the performance of self-regenerating Pt-based perovskite catalysts

Jarrige, I.*; 石井 賢司; 松村 大樹; 西畑 保雄; 吉田 雅洋*; 岸 浩史*; 谷口 昌司*; 上西 真里*; 田中 裕久*; 笠井 秀明*; et al.

ACS Catalysis, 5(2), p.1112 - 1118, 2015/02

 被引用回数:16 パーセンタイル:44.2(Chemistry, Physical)

Self-regenerating automotive catalysts owe their remarkable performance to the repeated motion of the precious metal atoms in and out of the perovskite lattice under fluctuating oxidizing and reducing conditions, preventing coalescence of the metal nanoparticles. Here we use resonant inelastic X-ray scattering to characterize the occupied and unoccupied Pt 5d states in two self-regenerating Pt-perovskite catalysts, CaTi$$_{0.95}$$Pt$$_{0.05}$$O$$_3$$ and CaZr$$_{0.95}$$Pt$$_{0.05}$$O$$_3$$. Upon reduction, the element and symmetry-specific charge excitation spectra reveal a sizeable hybridization between the Pt 5d and the Ti 3d or Zr 4d states at the interface between the nanoparticles and the perovskite, which involves the occupied states and is thus invisible in X-ray absorption spectra. A correlation is found between the strength of this d-band hybridization and the proportion of Pt nanoparticles that remain buried below the surface during reduction, indicating that the motion of the Pt atoms towards the surface is hindered by this hybridization specifically, rather than by the Pt-O bonding. These results provide direct evidence that the strength of the metal-metal d-band hybridization plays a pivotal role in determining the efficiency of self-regeneration in perovskite catalysts.

論文

In situ XAFS and HAXPES analysis and theoretical study of cobalt polypyrrole incorporated on carbon (CoPPyC) oxygen reduction reaction catalysts for anion-exchange membrane fuel cells

朝澤 浩一郎*; 岸 浩史*; 田中 裕久*; 松村 大樹; 田村 和久; 西畑 保雄; Saputro, A. G.*; 中西 寛*; 笠井 秀明*; Artyushkova, K.*; et al.

Journal of Physical Chemistry C, 118(44), p.25480 - 25486, 2014/11

 被引用回数:15 パーセンタイル:45.08(Chemistry, Physical)

Non-noble metal electrocatalysts not only are a solution to limited resources but also achieve higher efficiency for fuel cells, especially in alkaline media such as alkaline membrane fuel cells. Co-polypyrrole-based electrocatalysts provide high oxygen reduction reaction (ORR) reactivity, but the active sites and reaction mechanism have yet to be elucidated fully. In this study, ex situ and in situ synchrotron characterization and theoretical study have been combined to evaluate the ORR mechanism on two possible active sites consisting of Co coordinated with pyrrolic nitrogen and Co coordinated with pyridinic nitrogen.

論文

A Theoretical study of the reactivity of Cu$$_{2}$$O(111) surfaces; The Case of NO dissociation

岸 浩史*; Padama, A. A. B.*; Arevalo, R. L.*; Moreno, J. L. V.*; 笠井 秀明*; 谷口 昌司*; 上西 真里*; 田中 裕久*; 西畑 保雄

Journal of Physics; Condensed Matter, 24(26), p.262001_1 - 262001_5, 2012/07

 被引用回数:9 パーセンタイル:38.45(Physics, Condensed Matter)

NO分子解離に関するCu(111)とCu$$_{2}$$O(111)表面の電子状態を密度汎関数理論を用いた第一原理計算で比較した。NO分子の解離吸着反応の活性点として3回対称性のある銅原子及び酸素原子について注目した。銅原子と酸素原子の相互作用により、活性障壁が消失し、フェルミ準位直上に非占有状態が生じる。これらの知見はNO還元反応のための脱貴金属触媒の実現に向けて重要である。

論文

NO dissociation on Cu(111) and Cu$$_{2}$$O(111) surfaces; A Density functional theory based study

Padama, A. A. B.*; 岸 浩史*; Arevalo, R. L.*; Moreno, J. L. V.*; 笠井 秀明*; 谷口 昌司*; 上西 真里*; 田中 裕久*; 西畑 保雄

Journal of Physics; Condensed Matter, 24(17), p.175005_1 - 175005_6, 2012/05

 被引用回数:38 パーセンタイル:78.65(Physics, Condensed Matter)

Cu(111)表面とCu$$_{2}$$O(111)表面におけるNO分子の解離をスピン分極密度汎関数理論によって調べた。これはNOx還元反応のための銅をベースにした触媒の可能性を探るものである。吸着したNO分子の解離はどちらの表面でも起こる。酸化銅表面では遷移状態を経て反応が進むが、銅表面では途中でNO分子の脱離が起こる可能性があることが分かった。酸化銅の最表面に銅原子を配置することにより電子状態を変化させ、NO分子の吸着解離反応を制御できることが分かった。

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