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論文

Research on hydrogen safety technology utilizing the automotive catalyst

大野 瞳*; 竹中 啓恭*; 喜多 知輝*; 谷口 昌司*; 松村 大樹; 西畑 保雄; 日野 竜太郎; Reinecke, E.-A.*; 高瀬 和之*; 田中 裕久*

E-Journal of Advanced Maintenance (Internet), 11(1), p.40 - 45, 2019/05

Safety management technology of hydrogen gas is extremely important not only for nuclear power generation but also for future society. A brand-new passive autocatalytic recombiner (PAR) system utilizing the monolithic "intelligent catalyst" has been studied for the long-term storage of high-concentration radioactive materials related to the decommissioning of nuclear reactors. The monolith-type automotive catalyst showed high hydrogen conversion activity from a room temperature in a large scale reactor of REKO-4. It became clear that natural convection by reaction is greatly improved by roughening the cell density of the monolith catalyst especially under static environmental conditions such as in a storage container. Taking advantage of this superior catalytic property, we aim to complete the safety technology for storage containers at an early stage and advance the development of highly active catalyst from further low temperature.

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

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

Electrical and crystallographic study of an electrothermodynamic cycle for a waste heat recovery

Kim, J.*; 山中 暁*; 中島 啓*; 加藤 孝典*; Kim, J.*; Kim, Y.*; 福田 竜生; 吉井 賢資; 西畑 保雄; 馬場 将亮*; et al.

Advanced Sustainable Systems (Internet), 2(11), p.1800067_1 - 1800067_8, 2018/11

An innovative electrothermodynamic cycle (pyroelectric effect with an external electric field) was recently presented, which is based on temporal temperature variations in wasted heat from engine exhaust gas. In this paper, for further improvement, a generating mechanism of the cycle is investigated using in-operando time-resolved synchrotron X-ray diffraction with generating assessment. The polarizations of the sample are gained from both crystal/domain changes and simultaneous electrical measurements. Three types of materials are prepared: soft and hard types of lead zirconate titanate (PZT) and lead magnesium niobate-lead titanate (PMN-PT). Among them, PMN-PT has the highest generating power. When an external electric field is applied, the PMN-PT exhibits only 180$$^circ$$ domain rotations, whereas PZTs exhibit both 90$$^circ$$ and 180$$^circ$$ rotations. A strong driving force for 180$$^circ$$ rotation depresses rotations in other angles and increases polarization changes. The results show that the material development, which has only 180$$^circ$$ switching domains, has potential for use in the establishment of a high-efficiency waste heat recovery system.

論文

Temperature stability of PIN-PMN-PT ternary ceramics during pyroelectric power generation

Kim, J.*; 茂呂 拓哉*; Kim, J.*; 山中 暁*; 村山 一郎*; 加藤 孝典*; 中山 忠親*; 武田 雅敏*; 山田 昇*; 西畑 保雄; et al.

Journal of Alloys and Compounds, 768, p.22 - 27, 2018/11

 被引用回数:1 パーセンタイル:52.95(Chemistry, Physical)

Relaxor-based ternary Pb(In$$_{1/2}$$Nb$$_{1/2}$$)O$$_3$$-Pb(Mg$$_{1/3}$$Nb$$_{2/3}$$)O$$_3$$-PbTiO$$_3$$ (PIN-PMN-PT) ceramics near a morphotropic phase boundary were grown, and their electrical properties at various temperatures were investigated in the electrothermodynamic cycle for the future environment-friendly automotive applications. Structural disordering, depending on the PIN content, influenced the diffuse phase transition between the tetragonal and cubic structures and contributed to the power-generating behavior. The net power-generating energies (P$$_{net}$$) were 2.43-3.01 mW/cm$$^3$$ at temperatures above 200$$^circ$$C and were maintained at above 1 mW/cm$$^3$$ over a temperature range of approximately 100 degrees. Therefore, the PIN-PMN-PT system has a possibility of a wider usage temperature range, the disordering of the perovskite crystal structure can be controlled, and it will be a candidate for the application of pyroelectric energy conversion system.

論文

Nanoscale spatial analysis of clay minerals containing cesium by synchrotron radiation photoemission electron microscopy

吉越 章隆; 塩飽 秀啓; 小林 徹; 下山 巖; 松村 大樹; 辻 卓也; 西畑 保雄; 小暮 敏博*; 大河内 拓雄*; 保井 晃*; et al.

Applied Physics Letters, 112(2), p.021603_1 - 021603_5, 2018/01

 パーセンタイル:100(Physics, Applied)

放射光光電子顕微鏡(SR-PEEM)を人工的にCs吸着したミクロンサイズの風化黒雲母微粒子のピンポイント分析に適用した。絶縁物にもかかわらず、チャージアップの影響無しに構成元素(Si, Al, Cs, Mg, Fe)の空間分布を観察できた。Csが粒子全体に分布することが分かった。Cs M$$_{4,5}$$吸収端近傍のピンポイントX線吸収分光(XAS)から、1価の陽イオン状態(Cs$$^{+}$$)であることがわかった。さらに、Fe L$$_{2,3}$$吸収端の測定から、Feの価数状態を決定した。我々の結果は、サンプルの伝導性に左右されること無く、SR-PEEMがさまざまな環境試料に対するピンポイント化学分析法として利用可能であることを示すものである。

論文

Pyroelectric power generation with ferroelectrics (1-x)PMN-xPT

Kim, J.*; 山中 暁*; 中島 啓*; 加藤 孝典*; Kim, Y.*; 福田 竜生; 吉井 賢資; 西畑 保雄; 馬場 将亮*; 武田 雅敏*; et al.

Ferroelectrics, 512(1), p.92 - 99, 2017/08

 被引用回数:3 パーセンタイル:66.35(Materials Science, Multidisciplinary)

We have been investigating a novel electrothermodynamic cycle based on temporal temperature variations using the pyroelectric effect to utilize the waste heat as renewable energy. An improved generating performance with relaxer ferroelectric ceramics was achieved using 75Pb(Mg$$_{2/3}$$Nb$$_{1/3}$$)O$$_3$$-25PbTiO$$_3$$ which is well known for the high dielectric and pyroelectric properties. The potential was evaluated by using the hysteresis loops and generating properties are analyzed both in laboratory and engine dynamometer. Results showed 0.48 mW/cm$$^3$$ in engine dynamometer assessment, which is 3 times larger than the previous study using Pb(Zr,Ti)O$$_3$$.

論文

Relationship between the material properties and pyroelectric-generating performance of PZTs

山中 暁*; Kim, J.*; 中島 啓*; 加藤 孝典*; Kim, Y.*; 福田 竜生; 吉井 賢資; 西畑 保雄; 馬場 将亮*; 山田 昇*; et al.

Advanced Sustainable Systems (Internet), 1(3-4), p.1600020_1 - 1600020_6, 2017/04

我々がプロジェクトとして取り組んできている自動車排ガスを用いた温度変化発電に関し、変換素子の材料選定等に重要となる性能指数について、素子の物理量の温度変化の測定を行うことで調べた。測定結果を用い、これまで提案されていたいくつかの性能指数の温度変化を詳しく調べて比較することで、$$F_D$$と呼ばれる指数が最も発電量との相関が高いことを示した。この指数には唯一誘電正接($$tandelta$$)が含まれており、誘電体内での電気エネルギー損失が重要であることを示唆する結果となっている。

論文

${{it In situ}}$ X-ray absorption spectroscopy study on water formation reaction of palladium metal nanoparticle catalysts

松村 大樹; 谷口 昌司*; 田中 裕久*; 西畑 保雄

International Journal of Hydrogen Energy, 42(11), p.7749 - 7754, 2017/03

 被引用回数:1 パーセンタイル:87.11(Chemistry, Physical)

Proper management of hydrogen gas is extremely important for the safety security of nuclear power plants. Hydrogen removal by the water formation reaction on a catalyst is one of the candidates for creating hydrogen safety system. We observed in situ and real-time-resolved structure change of palladium metal nanoparticles during the water formation reaction by using X-ray absorption spectroscopy technique. The effect of carbon monoxide poisoning on catalytic activity was also studied. We have found that the creation of oxidized surface layer on palladium metal nanoparticles plays an important role of the water formation reaction process.

論文

Study on the behavior of halide ions on the Au(111) electrode surface in ionic liquids using surface X-ray scattering

田村 和久; 西畑 保雄

Journal of Physical Chemistry C, 120(29), p.15691 - 15697, 2016/07

 被引用回数:6 パーセンタイル:52.26(Chemistry, Physical)

これまでの多くの研究から、電気化学反応を精密に制御するためには、まさに電気化学反応が起きている場である電極/電解液界面で何が起きているかを、正確に知る必要があることが分かっている。イオン液体(IL)を電解質とした場合についても同様であり、これまでに様々な手法を用いて、界面の振る舞いの検討が行われてきている。しかしながら、これまでの研究において、ILに含まれる不純物が界面に与える影響について検討された例は少ない。水,ハロゲン化物イオン(X$$^{-}$$),アルカリ金属イオンなどが典型的な不純物であるが、これらは電気化学的に活性であることがわかっており、つまり、界面に存在していることを示している。したがって、より現実的にIL中での電気化学反応を理解する上で、IL中の不純物が界面でどのように振る舞い、界面の構造にどのような影響を与えるのかを理解することが重要である。そこで、本研究では、電気化学測定と表面X線散乱測定を組み合わせた手法により、ILに含まれるX$$^{-}$$が、電極/IL界面でどのような振る舞いをし、電極表面構造にどのような影響を与えるかを検討した。

論文

CO adsorption and decomposition on Pd/Al$$_{2}$$O$$_{3}$$ studied by time-resolved XAFS using dispersive optics

松村 大樹; 岡島 由佳*; 西畑 保雄

Journal of Physics; Conference Series, 712(1), p.012042_1 - 012042_4, 2016/06

 パーセンタイル:100

We have studied surface structural change of supported Pd metal nanoparticles caused by CO adsorption and following temperature increase by using ${{it in situ}}$ and time-resolved X-ray absorption fine structure technique with dispersive optics. CO adsorption on Pd metal nanoparticles at room temperature shows two types of adsorption behavior and the less stable CO which brings about surface expansion of Pd metal nanoparticles is desorbed just after temperature increase. Pd carbide layer is created at around 350 C by CO decomposition, which was clearly detected by the elongation of Pd-Pd interatomic distance and the increase of Debye-Waller factor and third cumulant.

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

Observation of all-in type tetrahedral displacements in nonmagnetic pyrochlore niobates

鳥越 秀平*; 石本 祐太朗*; 青石 優平*; 村川 寛*; 松村 大樹; 吉井 賢資; 米田 安宏; 西畑 保雄; 樹神 克明; 富安 啓輔*; et al.

Physical Review B, 93(8), p.085109_1 - 085109_5, 2016/02

 被引用回数:3 パーセンタイル:66.42(Materials Science, Multidisciplinary)

We observed all-in type Nb tetrahedral displacement in nonmagnetic pyrochlore niobates A$$_{2}$$Nb$$_{2}$$O$$_{7}$$ (A = Nd$$_{0.5}$$Ca$$_{0.5}$$ and Y$$_{0.5}$$Ca$$_{0.5}$$) through the analysis of the neutron pair distribution function and the extended X-ray absorption function spectroscopy. The all-in type Nb tetrahedral displacement, which has the character of a charge singlet state, is driven by the formation of the bonding orbital. The diffuse scattering in the X-ray diffraction, which has the resonant component in the Nb $$L$$3 edge, indicates that the all-in type Nb tetrahedral displacement has the periodicity with its short-range correlation.

論文

Precise observation of growth of surface oxide layer for Pd and Cu nanoparticles during oxidative/reductive gases cyclic flow studied by real-time-resolved XAFS spectroscopy

松村 大樹; 西畑 保雄; 岡島 由佳*

e-Journal of Surface Science and Nanotechnology (Internet), 14, p.48 - 52, 2016/00

We have demonstrated in situ and real-time-resolved X-ray absorption fine structure (XAFS) observation for oscillatory creation and removal reactions of surface oxide layer of Pd and Cu metal nanoparticles during cyclic flow of oxidative and reductive gases every 10 s. Pd and Cu $$K$$-edges XAFS spectra were collected at about 1-2 Hz. Precise observation of edge position was utilized for monitoring surface oxidation and reduction reactions. Reaction rate of surface oxide layer creation by NO for Pd metal nanoparticle is faster in the case of H$$_{2}$$/NO cyclic ow than in CO/NO. Fast and two-step surface oxidation and reduction reactions were revealed in Cu metal nanoparticles.

論文

Operando XAFS study of carbon supported Ni, NiZn, and Co catalysts for hydrazine electrooxidation for use in anion exchange membrane fuel cells

坂本 友和*; 松村 大樹; 朝澤 浩一郎*; Martinez, U.*; Serov, A.*; Artyushkova, K.*; Atanassov, P.*; 田村 和久; 西畑 保雄; 田中 裕久*

Electrochimica Acta, 163, p.116 - 122, 2015/05

 被引用回数:28 パーセンタイル:16.33(Electrochemistry)

Carbon supported Ni, Ni$$_{0.87}$$Zn$$_{0.13}$$, and Co hydrazine electrooxidation catalysts were synthesized by an impregnation/freeze-drying procedure followed by thermal annealing for use as anode catalyst of direct hydrazine hydrate fuel cells (DHFCs). The cell performance of DHFCs changed significantly when different catalysts were used as anode. Ammonia generation from anode outlet at open circuit voltage (OCV) condition was higher for Co/C than for Ni-based catalysts. To better understand the cause of different performance and selectivity of each anode catalyst, extensive ex-situ and operando characterization was carried out. Operando XAFS measurement of Ni-K and Co-$$K$$ edge shows the potential dependence of atomic structure of Ni/C, Ni$$_{0.87}$$Zn$$_{0.13}$$/C, and Co/C during hydrazine electrooxidation reaction.

論文

Development of new type passive autocatalytic recombiner, 1; Experimental study on degradation of catalyst

上地 優; 松村 大樹; 谷口 昌司*; 西畑 保雄; 田中 裕久*; 平田 慎吾*; 原 未来也; 日野 竜太郎

Proceedings of 23rd International Conference on Nuclear Engineering (ICONE-23) (DVD-ROM), 4 Pages, 2015/05

原子力発電所の過酷事故時においては、多量の水素が格納容器又は原子炉建屋へ放出される可能性がある。受動的触媒式再結合器(PAR)は、水素濃度緩和と安全な自己管理の最も有効な手段の一つである。既存のPARの性能向上のため、特に重量やサイズに着目した新形式のPARの開発を進めているところである。本研究では、自動車触媒の活性に対する水蒸気共存の影響について実験的な検討を実施した。その結果、水蒸気は、触媒反応の開始をわずかに遅らせる傾向があるものの、定常的な影響はないことを明らかにした。

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:8 パーセンタイル:61.22(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

Real-time-resolved X-ray absorption fine structure spectroscopy for cesium adsorption on some clay minerals

松村 大樹; 小林 徹; 宮崎 有史; 岡島 由佳*; 西畑 保雄; 矢板 毅

Clay Science, 18(4), p.99 - 105, 2014/12

Real-time-resolved observation by using X-ray absorption fine structure spectroscopy was employed in order to study the interaction between dropped water and a mixture of clay minerals and cesium chloride. Change of X-ray absorption spectra were used for the evaluation of amount and chemical state of cesium compounds. For sericite and illite clays, relatively long lifetime of hydrated cesium ions was observed before adsorption on clay minerals. On the other hand, for vermiculite, kaolinite and zeolite clays, hydrated cesium ions were not intensely observed due to short reaction time between hydrated cesium ions and the clay minerals. The electronic configuration of cesium adsorbed on the vermiculite clay is different from that of cesium adsorbed on the other clay minerals. Real-time-resolved X-ray absorption fine structure spectroscopy observation is expected to be widely used for the study of the cesium adsorption on many clay minerals.

論文

Local structure around cesium in montmorillonite, vermiculite and zeolite under wet condition

辻 卓也; 松村 大樹; 小林 徹; 鈴木 伸一; 吉井 賢資; 西畑 保雄; 矢板 毅

Clay Science, 18(4), p.93 - 97, 2014/12

We have observed the local structure around cesium in silicate minerals under wet and dry conditions by using X-ray absorption fine structure (XAFS) technique at Cs ${it K}$-edge. The measurements under wet and dry conditions simulated changes of the actual environment. High transmission ability at Cs ${it K}$-edge provides XAFS measurement under various conditions. Montmorillonite, vermiculite, and zeolite were employed for the study. Vermiculite was obtained by wet classification of the actual soil at Fukushima. The result of XAFS measurement shows that water molecules in interlayer position are removed by cesium adsorption in the interlayer site of vermiculite. Cesium ion was adsorbed on one side of the interlayer site of swelled montmorillonite under wet condition. On the other hand, water molecules were not coordinated with cesium ion in the zeolite even in the case of wet condition.

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:11 パーセンタイル:46.5(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

Development of new type passive autocatalytic recombiner, 1; Characterization of monolithic catalyst

上地 優; 谷口 昌司*; 西畑 保雄; 永石 隆二; 田中 裕久*; 平田 慎吾*; 原 未来也; 日野 竜太郎

Proceedings of 2nd International Conference on Maintenance Science and Technology (ICMST-Kobe 2014), p.87 - 88, 2014/11

原子炉におけるSAMのひとつである水素影響緩和のため、新形式の静的触媒式再結合器が開発されている。これは、重量削減や水素処理性能、環境耐性及び製品品質の向上のため、自動車用のモノリス担体触媒をもとに開発が進められている。本研究では、触媒の基本性能を明らかにするため水素再結合反応における活性化エネルギーを評価した。また、$$gamma$$線照射による劣化に関する評価も併せて実施した。実験結果から、量論組成ガス供給において、活性化エネルギーは5.7kJ/molと算出された。また、1.0MGyまでの$$gamma$$線照射では、劣化が生じることはなく、むしろ触媒活性を増加させる効果があることが分かった。

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