発表論文

2018年

"Tin-palladium supported on alumina as a highly active and selective catalyst for hydrogenation of nitrate in actual groundwater polluted with nitrate"
Jun Hirayama, Yuichi Kamiya
Catal. Sci. Technol., 8 (2018) 4985-4993. DOI: 10.1039/C8CY00730F
Abstract

We developed Sn0.5Pd/Al2O3 showing high activity and high selectivity to gaseous products towards the hydrogenation of NO3- with H2 in aqueous NO3- solutions via precise control of the Sn/Pd molar ratio. For the catalyst with the optimum Sn/Pd molar ratio, the surface concentration of adsorbed nitrogen on the Pd sites is thought to be high and that of the adsorbed hydrogen on the Pd sites is thought to be low. This is due to the abundant supply of NO2- for the Pd sites and the prompt consumption of adsorbed H on the Pd sites for reduction of the oxidized Sn sites formed by the reduction of NO3-, respectively, leading to the high selectivity to gaseous products. Although the catalytic performance of Sn0.5Pd/Al2O3, like that of Cu0.5Pd/Al2O3, was lower in groundwater, the decrease for Sn0.5Pd/Al2O3 was less than that for Cu0.5Pd/Al2O3. Nitrate in the groundwater polluted with 0.4 mmol dm-3 (250 cm3) of NO3- was completely reduced at 298 K in 24 h with a selectivity for gaseous products of around 90% in the presence of 10 mg of Sn0.5Pd/Al2O3, whereas it took 60 h in the presence of Cu0.5Pd/Al2O3, and the selectivity for gaseous products was around 75%. However, both catalysts showed comparable high activity and high selectivity in aqueous NO3- solutions. When reactions were performed in aqueous NO3- solutions containing other anions (Cl-, SO42-, and SiOxn-) present in the groundwater, Cl- had the largest negative impact but it had a smaller impact in the presence of Sn0.5Pd/Al2O3 than it did in the presence of Cu0.5Pd/Al2O3. On the basis of adsorption isotherms for Cl- and kinetics analysis of the hydrogenation of NO3-, it was concluded that Sn0.5Pd/Al2O3 had less affinity for Cl- and a strong affinity for NO3- on the Sn sites, leading to its superior catalytic performance in groundwater.



"Determination of acid site location in dealuminated MCM-68 by Al-27 MQMAS NMR and FT-IR spectroscopy with probe molecules"
Ryoichi Otomo, Toshiki Nishitoba, Rota Ogusa, Yusuke Kunitake, Yuichi Kamiya, Takashi Tatsumi, Toshiyuki Yokoi
J. Phys. Chem. C, 122 (2018) 1180-1191. DOI: 10.1021/acs.jpcc.7b09576



学会発表

2018年度

第67回研究発表会(5月22日〜23日、東京)
(口頭発表)大友 “Hf含有ゼオライトベータのフッ素を用いるポスト合成”
(ポスター発表)中村 “フッ素を含有したHf-Betaの酸塩基触媒特性”
International Symposium focusing on Advancement and Prospect of Catalysis Science & Technology(Pre-symposium of ISHHC 18)(7月25日〜27日、シドニー)
(招待講演)大友 “Post-synthesis of highly active Hf-Beta zeolite assisted by NH4F: a new insight into the formation of active Lewis acid sites for MPV reduction”
日本化学会北海道支部 2018年夏季研究発表会(7月21日、北見)
(口頭発表)橋本 “異元素置換したSrFeO3による低級炭化水素酸化”
(口頭発表)長尾 “チタン原子価が制御された低原子価チタン酸化物の触媒特性”
(口頭発表)藤元 “さまざまな金属酸窒化物の塩基触媒特性”
(口頭発表)大友 “BPO4触媒を用いた気相プロパンジオール脱水反応における水蒸気添加効果”
(口頭発表)神谷 “水中硝酸イオン還元反応に対するスズ-パラジウム触媒と銅-パラジウム触媒の触媒特性比較”
Pre-conference of TOCAT8 and the 5th International Symposium of Institute for Catalysis(8月3日〜4日、札幌)
(口頭発表)金 “Adjacent acid-base pair sites on silica surface constructed by hydrolysis of pre-anchored amide fixed on silica”
TOCAT 8(8月5日〜9日、横浜)
(口頭発表)平山 “Catalytic reduction of nitrate in water toward purification of real groundwater”
(ポスター発表)金 “Adjacent acid-base pair sites on silica surface constructed by hydrolysis of pre-anchored amide”
ZMPC2018(8月5日〜9日、横浜)
(口頭発表)大友 “Determination of Acid Site Location in Dealuminated MCM-68 with 12-10-10-ring Structure by 27Al MQMAS NMR and FT-IR Spectroscopy with Probe Molecules”
第122回触媒討論会(9月26日〜28日、函館)
(口頭発表)長尾 “固相法で合成した低原子価チタン酸化物の酸塩基触媒特性”
(口頭発表)橋本 “Bサイトを部分 置換したSrFeO3の酸化触媒特性”
(口頭発表)金 “アミドの加水分 解を利用するシリカ上に構築した酸点-塩基点の隣接距離制御”
(口頭発表)小船 “担持ニッケル触媒による水中硝酸イオン還元反応の速度論解析”
(口頭発表)十川 “塩化物イオン存在下での水中アンモニウムイオンのオゾン接触酸化分解におけるクロラミン類の生成挙動”
(口頭発表)大友 “Hf-βのポスト合成におけるフッ化アンモニウム添加効果”
(口頭発表)祝迫 “1,2-プロパンジオールの脱水反応に高活性を示す金属リン酸塩触媒の探索”
第48回石油・石油化学討論会(10月17日〜18日、東京)
(口頭発表)神谷 “12-モリブドリン酸触媒上でのメタクロレイン酸化反応における添加水蒸気の役割”
(口頭発表)大友 “メタロケイ酸塩ゼオライトのポスト合成におけるフッ素添加効果”
第34回ゼオライト研究発表会(11月29日〜30日、函館)
(口頭発表)大友 “メタロケイ酸塩ゼオライトベータの合成におけるフッ素添加効果”
(口頭発表)中村 “フッ素を添加してポスト合成したHf-Betaの触媒特性”
2018年度触媒学会北海道支部 北見地区講演会(12月21日、北見)
(招待講演)大友 “バイオマス変換を志向した含酸素官能基の自在な変換を可能にする高活性固体酸触媒の開発”

表彰

2018年3月
第121回触媒討論会 学生ポスター発表賞
金源兌 ”アミドの加水分解による近接した酸点-塩基点の構築”
2018年8月
TOCAT8 Best Poster Award
金源兌 "Adjacent acid-base pair sites on silica surface constructed by hydrolysis of pre-anchored amide”