Unravelling the cohesion in complex hydrides for materials exploration

• Project/Area Number: 26820312
• Research Category: Grant-in-Aid for Young Scientists (B)
• Allocation Type: Multi-year Fund
• Research Field: Structural/Functional materials
• Research Institution: Tohoku University
• Principal Investigator: Takagi Shigeyuki 東北大学, 金属材料研究所, 助教 (50409455)
• Project Period (FY): 2014-04-01 – 2016-03-31
• Project Status: Completed (Fiscal Year 2015)
• Budget Amount: ¥3,770,000 (Direct Cost: ¥2,900,000、Indirect Cost: ¥870,000); Fiscal Year 2015: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000); Fiscal Year 2014: ¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
• Keywords: 錯体水素化物 / 水素 / 遷移金属 / 化学結合 / 配位子場 / 電気陰性度 / 18電子則 / 水素貯蔵

Outline of Final Research Achievements

Complex hydrides have attracted attention for many years because of their many potential functionalities, including hydrogen storage, fast-ionic conductivity and superconductivity. In this study, by means of a combined theoretical/experimental approach, we investigated the cohesion in complex hydrides in order to obtain knowledge for exploration of new materials. We developed several guidelines for materials exploration and successfully synthesized several new complex hydrides with high hydrogen density.

Research Products

• [Journal Article] Metallic Intermediate Hydride Phase of LaMg2Ni with Ni-H Covalent Bonding: Precursor State for Complex Hydride Formation (2016)
  • Author(s): K. Miwa, T. Sato, M. Matsuo, K. Ikeda, T. Otomo, S. Deledda, B. C. Hauback, G. Li, S. Takagi, S. Orimo
  • Journal Title: J. Phys. Chem. C Volume: 120 Issue: 11 Pages: 5926-5931
  • DOI: 10.1021/acs.jpcc.6b00341
  • Peer Reviewed / Int'l Joint Research / Acknowledgement Compliant
• [Journal Article] Extending the Applicability of the Goldschmidt Tolerance Factor to Arbitrary Ionic Compounds (2016)
  • Author(s): T. Sato, S. Takagi, S. Deledda, B. C. Hauback, S. Orimo
  • Journal Title: Sci. Rep. Volume: 6 Issue: 1 Pages: 23592-23592
  • DOI: 10.1038/srep23592
  • Peer Reviewed / Open Access / Int'l Joint Research / Acknowledgement Compliant
• [Journal Article] True boundary for the formation of homoleptic transition-metal hydride complexes (2015)
  • Author(s): S. Takagi, Y. Iijima, T. Sato, H. Saitoh, K. Ikeda, T. Otomo, K. Miwa, T. Ikeshoji, K. Aoki, S. Orimo
  • Journal Title: Angewandte Chemie International Edition Volume: 54 Issue: 19 Pages: 5650-5653
  • DOI: 10.1002/anie.201500792
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] Recent progress in hydrogen-rich materials from the perspective of bonding flexibility of hydrogen (2015)
  • Author(s): S. Takagi, S. Orimo
  • Journal Title: Scripta Materialia Volume: 109 Pages: 1-5
  • DOI: 10.1016/j.scriptamat.2015.07.024
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] Complex transition metal hydrides incorporating ionic hydrogen: Synthesis and characterization of Na2Mg2FeH8 and Na2Mg2RuH8 (2015)
  • Author(s): T.D. Humphries, S. Takagi, G Li, M. Matsuo, T. Sato, M.H. Sorby, S. Deledda, B.C. Hauback, S, Orimo
  • Journal Title: Journal of Alloys and Compounds Volume: in press Pages: S347-S352
  • DOI: 10.1016/j.jallcom.2014.12.113
  • Peer Reviewed
• [Journal Article] Multi-Phonon Excitations in Fe 2p RIXS on Mg2FeH6 (2015)
  • Author(s): K. Kurita, D. Sekiba, I. Harayama, K. Chito, Y. Harada, H. Kiuchi, M. Oshima, S. Takagi, M. Matsuo, R. Sato, K. Aoki, S. Orimo
  • Journal Title: Journal of the Physical Society of Japan Volume: 84 Issue: 4 Pages: 043201-043201
  • DOI: 10.7566/jpsj.84.043201
  • Peer Reviewed
• [Journal Article] Enhanced tunability of thermodynamic stability of complex hydride by the incorporation of H- anions (2014)
  • Author(s): S. Takagi, T.D. Humphries, K. Miwa, S. Orimo
  • Journal Title: Applied Physics Letters Volume: 104 Issue: 20
  • DOI: 10.1063/1.4878775
  • Peer Reviewed / Open Access / Acknowledgement Compliant
• [Journal Article] Li4FeH6: iron-containing complex hydride with high gravimetric hydrogen density (2014)
  • Author(s): H. Saitoh, S. Takagi, M. Matsuo, Y. Iijima, N. Endo, K. Aoki, S. Orimo
  • Journal Title: APL Materials Volume: 2 Issue: 7 Pages: 076103-076103
  • DOI: 10.1063/1.4886219
  • Peer Reviewed / Open Access / Acknowledgement Compliant
• [Journal Article] Raman and Infrared Spectroscopic Studies on Li₄RuH₆ Combined with First-Principles Calculations (2014)
  • Author(s): T. Sato, S. Takagi, M. Matsuo, K. Aoki, S. Deledda, B.C. Hauback, S. Orimo
  • Journal Title: MATERIALS TRANSACTIONS Volume: 55 Issue: 8 Pages: 1117-1121
  • DOI: 10.2320/matertrans.MG201403
  • NAID: 130004455350
  • ISSN: 1345-9678, 1347-5320
  • Peer Reviewed / Open Access / Acknowledgement Compliant
• [Journal Article] Magnesium ion dynamics in Mg(BH4)2(1-x)X2x (X=Cl or AlH4) from first-principles molecular dynamics simulations (2014)
  • Author(s): T. Ikeshoji, E.Tsuchida, S.Takagi, M.Matsuo, and S.Orimo
  • Journal Title: RSC Advances Volume: 4 Issue: 3 Pages: 1366-1370
  • DOI: 10.1039/c3ra42453g
  • Peer Reviewed
• [Presentation] 水素 9 配位錯イオンを含む新たな錯体水素化物の理論探索と合成 (2016)
  • Author(s): 髙木成幸, 齋藤寛之, 佐藤豊人, 飯島祐樹, 池田一貴, 松尾元彰, 池庄司民夫, 三輪和利, 大友季哉, 折茂慎一
  • Organizer: 日本金属学会2016年春期（第158回）大会
  • Place of Presentation: 東京
  • Year and Date: 2016-03-23
• [Presentation] 中性子非弾性散乱を用いたAl系錯体水素化物におけるAl－H結合の振動モード観測 (2016)
  • Author(s): 佐藤豊人 , A.J. Ramirez-Cuesta, L. Daemen, Y. Cheng, 髙木成幸, 富安啓輔, 折茂慎一
  • Organizer: 日本金属学会2016年春期（第158回）大会
  • Place of Presentation: 東京
  • Year and Date: 2016-03-23
• [Presentation] LaMg2Ni-H系の金属中間相LaMg2Ni4.6に対する第一原理計算 (2016)
  • Author(s): 三輪和利, 佐藤豊人, 松尾元彰, 池田一貴, 大友季哉, S. Deledda, B.C. Hauback, 李関喬, 髙木成幸, 折茂慎一
  • Organizer: 日本金属学会2016年春期（第158回）大会
  • Place of Presentation: 東京
  • Year and Date: 2016-03-23
• [Presentation] 第一原理計算と量子ビームによる高密度水素化物探索 (2016)
  • Author(s): 高木成幸, 齋藤寛之, 池田一貴, 大友季哉, 折茂慎一
  • Organizer: 第7回MLFシンポジウム
  • Place of Presentation: つくば
  • Year and Date: 2016-03-15
  • Invited
• [Presentation] Exploration of hydrogen-rich materials (2016)
  • Author(s): S. Takagi, Y. Iijima, T. Sato, H. Saitoh, K. Ikeda, T. Otomo, K. Miwa, T. Ikeshoji, K. Aoki, S. Orimo
  • Organizer: 10th International Symposium Hydrogen & Energy
  • Place of Presentation: 蔵王
  • Year and Date: 2016-02-21
  • Int'l Joint Research
• [Presentation] Syntheses of novel hydrides under high pressuere (2016)
  • Author(s): H. Saitoh, S. Takagi, K. Aoki, S. Orimo
  • Organizer: 10th International Symposium Hydrogen & Energy
  • Place of Presentation: 蔵王
  • Year and Date: 2016-02-21
  • Int'l Joint Research
• [Presentation] Crystal structure indicator: The ionic filling fraction of hydrides with arbitrary arranged ionic components (2016)
  • Author(s): T. Sato, S. Takagi, S. Deledda, B. C. Hauback, S. Orimo
  • Organizer: 10th International Symposium Hydrogen & Energy
  • Place of Presentation: 蔵王
  • Year and Date: 2016-02-21
  • Int'l Joint Research
• [Presentation] How cations move in boron-hydride electrolytes: First-principals molecular dynamics (2016)
  • Author(s): T. Ikeshoji, A. Unemoto, S. Takagi, M. Matsuo, S. Orimo
  • Organizer: 10th International Symposium Hydrogen & Energy
  • Place of Presentation: 蔵王
  • Year and Date: 2016-02-21
  • Int'l Joint Research
• [Presentation] 高水素密度材料の理論探索 (2015)
  • Author(s): 髙木成幸, 齋藤寛之, 佐藤豊人, 飯島祐樹, 池庄司民夫, 青木勝敏, 折茂 慎一
  • Organizer: 第56回高圧討論会
  • Place of Presentation: 広島
  • Year and Date: 2015-11-10
  • Invited
• [Presentation] 放射光その場観察を利用した金属錯体水素化物の高温高圧合成研究 (2015)
  • Author(s): 齋藤寛之, 髙木成幸, 飯島祐樹, 佐藤豊人, 松尾元彰, 青木勝敏, 折茂 慎一
  • Organizer: 第56回高圧討論会
  • Place of Presentation: 広島
  • Year and Date: 2015-11-10
  • Invited
• [Presentation] 遷移金属錯イオンの対称性と水素の配位子場効果 (2015)
  • Author(s): 髙木 成幸, 齋藤 寛之、三輪 和利、折茂 慎一
  • Organizer: 第2回水素化物に関わる次世代学術・応用展開研究会
  • Place of Presentation: 金沢
  • Year and Date: 2015-10-22
• [Presentation] 新規水素化物の結晶構造を決定するプロセス (2015)
  • Author(s): 佐藤豊人, 高木 成幸, S. Deledda, B.C. Hauback, 折茂 慎一
  • Organizer: 第2回水素化物に関わる次世代学術・応用展開研究会
  • Place of Presentation: 金沢
  • Year and Date: 2015-10-22
• [Presentation] クロム系高配位錯イオンを含む錯体水素化物の理論探索と合成 (2015)
  • Author(s): 髙木成幸, 飯島祐樹, 佐藤豊人, 齋藤寛之, 池田一貴, 大友季哉, 三輪和利, 池庄司民夫, 青木勝敏, 折茂慎一
  • Organizer: 日本金属学会2015年秋期（第157回）大会
  • Place of Presentation: 福岡
  • Year and Date: 2015-09-16
• [Presentation] 高密度水素化物実現を目指した高温高圧合成研究 (2015)
  • Author(s): 齋藤寛之, 髙木成幸, 青木勝敏, 折茂慎一
  • Organizer: 日本金属学会2015年秋期（第157回）大会
  • Place of Presentation: 福岡
  • Year and Date: 2015-09-16
• [Presentation] 結晶構造解析における最適な単位胞及び組成比決定のための指標の構築 (2015)
  • Author(s): 佐藤豊人, 髙木成幸, S. Deledda, B.C. Hauback, 折茂慎一
  • Organizer: 日本金属学会2015年秋期（第157回）大会
  • Place of Presentation: 福岡
  • Year and Date: 2015-09-16
• [Presentation] 塩化物イオンを含むAl系錯体水素化物の脱水素化反応 (2015)
  • Author(s): 佐藤豊人, 赤城拓馬, 髙木成幸, Stefano Deledda, B. C. Hauback, 折茂 慎一
  • Organizer: 日本金属学会2015年春期（第156回）大会
  • Place of Presentation: 東京大学（東京都目黒区）
  • Year and Date: 2015-03-18 – 2015-03-20
• [Presentation] 8族元素を含む錯体水素化物の合成と結晶構造及び、格子振動 (2014)
  • Author(s): 尾形昂洋, 佐藤豊人, 髙木成幸, 齋藤寛之, 飯島祐樹, 青木勝敏, 折茂慎一
  • Organizer: 日本金属学会2014年秋期（第155回）大会
  • Place of Presentation: 名古屋大学（愛知県名古屋市）
  • Year and Date: 2014-09-24 – 2014-09-26
• [Presentation] V80Ti20で観察された水素吸蔵量の回復現象に及ぼす水素化温度、添加元素の効果 (2014)
  • Author(s): H. Kim, 德尾高宏, 榊浩司, 髙木成幸, 榎浩利, 岩瀬謙二, 折茂慎一, 中村優美子
  • Organizer: 日本金属学会2014年秋期（第155回）大会
  • Place of Presentation: 名古屋大学（愛知県名古屋市）
  • Year and Date: 2014-09-24 – 2014-09-26
• [Presentation] 固相メタセシス反応によるAl系錯体水素化物の合成と結晶構造解析 (2014)
  • Author(s): 佐藤豊人, 赤城拓馬, 髙木成幸, S. Deledda, B. C. Hauback, 折茂慎一
  • Organizer: 日本金属学会2014年秋期（第155回）大会
  • Place of Presentation: 名古屋大学（愛知県名古屋市）
  • Year and Date: 2014-09-24 – 2014-09-26
• [Presentation] 水素イオンを含む遷移金属錯体水素化物:材料探索ならびに安定性制御 (2014)
  • Author(s): 髙木成幸, T.D. Humphries, 三輪和利, 折茂慎一
  • Organizer: 日本金属学会2014年秋期（第155回）大会
  • Place of Presentation: 名古屋大学（愛知県名古屋市）
  • Year and Date: 2014-09-24 – 2014-09-26
• [Presentation] Theoretical exploration and syntheses of complex transition metal hydrides with high gravimetric hydrogen density (2014)
  • Author(s): S. Takagi, H. Saitoh, T. Ikeshoji, K. Aoki, S. Orimo
  • Organizer: International Symposium on Metal-Hydrogen Systems 2014 (MH2014)
  • Place of Presentation: Manchester, UK
  • Year and Date: 2014-07-21 – 2014-07-25
• [Presentation] Complex transition metal hydrides incorporating covalent and ionic hydrogen (2014)
  • Author(s): T.D. Humphries, G. Li, M. Matsuo, S. Takagi, M.H. Sørby, T. Sato, B.C. Hauback, S. Orimo
  • Organizer: International Symposium on Metal-Hydrogen Systems 2014 (MH2014)
  • Place of Presentation: Manchester, UK
  • Year and Date: 2014-07-21 – 2014-07-25
• [Presentation] Synthesis, crystal structure and dehydrogenation reaction on a mixed alkali and alkaline-earth metal alanate LiCa(AlH4)3 (2014)
  • Author(s): T. Sato, S. Takagi, S. Deledda, B.C. Hauback, S. Orimo
  • Organizer: International Symposium on Metal-Hydrogen Systems 2014 (MH2014)
  • Place of Presentation: Manchester, UK
  • Year and Date: 2014-07-21 – 2014-07-25
• [Book] The lightest metals: Science and technology from lithium to calcium (2015)
  • Author(s): H. Saito, S. Takagi, K. Aoki, S. Orimo
  • Total Pages: 8
  • Publisher: John Wiley & Sons
• [Book] 水素利用技術集成 vol.4 高効率貯蔵技術、水素社会構築を目指して (2014)
  • Author(s): 池田一貴, 髙木成幸, 大友季哉, 折茂慎一
  • Total Pages: 354
  • Publisher: NTS出版