Heterogeneous catalytic and chemical looping routes to N2 activation: general discussion

Fatima Abi Ghaida; Katharina Brinkert; Yongli Cai; C. Richard A. Catlow; Hsin Yi Tiffany Chen; Ping Chen; Jean Philippe Dacquin; Angela Daisley; Joseph El-Kadi; Wenbo Gao; Jianping Guo; Justin S.J. Hargreaves; Michael D. Higham; Patrick L Holland; Hideo Hosono; Gavin J. Irvine; John T.S. Irvine; Manpreet Kaur; Yoji Kobayashi; Said Laassiri; Luc Liedtke; Douglas R. MacFarlane; Josh Makepeace; Ian J. McPherson; Vineet Mishra; Pinkie Ntola; Shiho Otomo; Jonas C. Peters; Yasushi Sekine; Zhangjie Shi; Carsten Sievers; Ifan E.L. Stephens; Tim Sudmeier; Laura Torrente Murciano; Deniz Uner; Qianru Wang; Yaolin Wang; Olivia Westhead; Lukman Yusuf; Xin Zeng

doi:10.1039/d3fd90010j

Heterogeneous catalytic and chemical looping routes to N₂ activation: general discussion

Fatima Abi Ghaida, Katharina Brinkert, Yongli Cai, C. Richard A. Catlow, Hsin Yi Tiffany Chen, Ping Chen, Jean Philippe Dacquin, Angela Daisley, Joseph El-Kadi, Wenbo Gao, Jianping Guo, Justin S.J. Hargreaves, Michael D. Higham, Patrick L Holland, Hideo Hosono, Gavin J. Irvine, John T.S. Irvine, Manpreet Kaur, Yoji Kobayashi, Said LaassiriLuc Liedtke, Douglas R. MacFarlane, Josh Makepeace, Ian J. McPherson, Vineet Mishra, Pinkie Ntola, Shiho Otomo, Jonas C. Peters, Yasushi Sekine, Zhangjie Shi, Carsten Sievers, Ifan E.L. Stephens, Tim Sudmeier, Laura Torrente Murciano, Deniz Uner, Qianru Wang, Yaolin Wang, Olivia Westhead, Lukman Yusuf, Xin Zeng

School of Chemistry

Research output: Contribution to journal › Comment / Debate › Other › peer-review

Abstract

Justin S. J. Hargreaves opened discussion of the introductory lecture by Hideo Hosono: In the case of conventionally supported ruthenium catalysed ammonia synthesis there is a strong influence of particle size which can be associated with the expression of B5 active sites. In the case of electride supported ruthenium is the nature of any structure sensitivity different?

Hideo Hosono responded: Ru B5 sites exhibit high activity. I think this is also true for the electride support. The role of the electride is promotion of electrons to the N 2 absorbed on the Ru, leading to N2 dissociation. One thing to add: LaRuSi is a layered crystal. Ru atoms form a planar unit, with no B5 site, but this material works well. The turnover frequency (TOF) is 600 times higher than that of pure Ru powder. Density functional theory (DFT) calculations revealed that the dissociation of N2 occurs easily on the exposed Ru plane of LaRuSi. A systematic study provides rm evidence that layered Ru with a negative charge in LnRuSi is a new type of active site that differs signicantly from B5sites.1 I think the active site is not restricted to B5 sites.

Original language	English
Pages (from-to)	198-230
Number of pages	33
Journal	Faraday Discussions
Volume	243
DOIs	https://doi.org/10.1039/d3fd90010j
Publication status	Published - 26 Jun 2023

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Abi Ghaida, F., Brinkert, K., Cai, Y., Catlow, C. R. A., Chen, H. Y. T., Chen, P., Dacquin, J. P., Daisley, A., El-Kadi, J., Gao, W., Guo, J., Hargreaves, J. S. J., Higham, M. D., Holland, PL., Hosono, H., Irvine, G. J., Irvine, J. T. S., Kaur, M., Kobayashi, Y., ... Zeng, X. (2023). Heterogeneous catalytic and chemical looping routes to N₂ activation: general discussion. Faraday Discussions, 243, 198-230. https://doi.org/10.1039/d3fd90010j

@article{38cc339ac037458daf9eca3c8c84c340,

title = "Heterogeneous catalytic and chemical looping routes to N2 activation: general discussion",

abstract = "Justin S. J. Hargreaves opened discussion of the introductory lecture by Hideo Hosono: In the case of conventionally supported ruthenium catalysed ammonia synthesis there is a strong influence of particle size which can be associated with the expression of B5 active sites. In the case of electride supported ruthenium is the nature of any structure sensitivity different?Hideo Hosono responded: Ru B5 sites exhibit high activity. I think this is also true for the electride support. The role of the electride is promotion of electrons to the N 2 absorbed on the Ru, leading to N2 dissociation. One thing to add: LaRuSi is a layered crystal. Ru atoms form a planar unit, with no B5 site, but this material works well. The turnover frequency (TOF) is 600 times higher than that of pure Ru powder. Density functional theory (DFT) calculations revealed that the dissociation of N2 occurs easily on the exposed Ru plane of LaRuSi. A systematic study provides rm evidence that layered Ru with a negative charge in LnRuSi is a new type of active site that differs signicantly from B5sites.1 I think the active site is not restricted to B5 sites.",

author = "{Abi Ghaida}, Fatima and Katharina Brinkert and Yongli Cai and Catlow, {C. Richard A.} and Chen, {Hsin Yi Tiffany} and Ping Chen and Dacquin, {Jean Philippe} and Angela Daisley and Joseph El-Kadi and Wenbo Gao and Jianping Guo and Hargreaves, {Justin S.J.} and Higham, {Michael D.} and Patrick L Holland and Hideo Hosono and Irvine, {Gavin J.} and Irvine, {John T.S.} and Manpreet Kaur and Yoji Kobayashi and Said Laassiri and Luc Liedtke and MacFarlane, {Douglas R.} and Josh Makepeace and McPherson, {Ian J.} and Vineet Mishra and Pinkie Ntola and Shiho Otomo and Peters, {Jonas C.} and Yasushi Sekine and Zhangjie Shi and Carsten Sievers and Stephens, {Ifan E.L.} and Tim Sudmeier and {Torrente Murciano}, Laura and Deniz Uner and Qianru Wang and Yaolin Wang and Olivia Westhead and Lukman Yusuf and Xin Zeng",

year = "2023",

month = jun,

day = "26",

doi = "10.1039/d3fd90010j",

language = "English",

volume = "243",

pages = "198--230",

journal = "Faraday Discussions",

issn = "1359-6640",

publisher = "The Royal Society of Chemistry",

}

Abi Ghaida, F, Brinkert, K, Cai, Y, Catlow, CRA, Chen, HYT, Chen, P, Dacquin, JP, Daisley, A, El-Kadi, J, Gao, W, Guo, J, Hargreaves, JSJ, Higham, MD, Holland, PL, Hosono, H, Irvine, GJ, Irvine, JTS, Kaur, M, Kobayashi, Y, Laassiri, S, Liedtke, L, MacFarlane, DR, Makepeace, J, McPherson, IJ, Mishra, V, Ntola, P, Otomo, S, Peters, JC, Sekine, Y, Shi, Z, Sievers, C, Stephens, IEL, Sudmeier, T, Torrente Murciano, L, Uner, D, Wang, Q, Wang, Y, Westhead, O, Yusuf, L & Zeng, X 2023, 'Heterogeneous catalytic and chemical looping routes to N₂ activation: general discussion', Faraday Discussions, vol. 243, pp. 198-230. https://doi.org/10.1039/d3fd90010j

TY - JOUR

T1 - Heterogeneous catalytic and chemical looping routes to N2 activation

T2 - general discussion

AU - Abi Ghaida, Fatima

AU - Brinkert, Katharina

AU - Cai, Yongli

AU - Catlow, C. Richard A.

AU - Chen, Hsin Yi Tiffany

AU - Chen, Ping

AU - Dacquin, Jean Philippe

AU - Daisley, Angela

AU - El-Kadi, Joseph

AU - Gao, Wenbo

AU - Guo, Jianping

AU - Hargreaves, Justin S.J.

AU - Higham, Michael D.

AU - Holland, Patrick L

AU - Hosono, Hideo

AU - Irvine, Gavin J.

AU - Irvine, John T.S.

AU - Kaur, Manpreet

AU - Kobayashi, Yoji

AU - Laassiri, Said

AU - Liedtke, Luc

AU - MacFarlane, Douglas R.

AU - Makepeace, Josh

AU - McPherson, Ian J.

AU - Mishra, Vineet

AU - Ntola, Pinkie

AU - Otomo, Shiho

AU - Peters, Jonas C.

AU - Sekine, Yasushi

AU - Shi, Zhangjie

AU - Sievers, Carsten

AU - Stephens, Ifan E.L.

AU - Sudmeier, Tim

AU - Torrente Murciano, Laura

AU - Uner, Deniz

AU - Wang, Qianru

AU - Wang, Yaolin

AU - Westhead, Olivia

AU - Yusuf, Lukman

AU - Zeng, Xin

PY - 2023/6/26

Y1 - 2023/6/26

N2 - Justin S. J. Hargreaves opened discussion of the introductory lecture by Hideo Hosono: In the case of conventionally supported ruthenium catalysed ammonia synthesis there is a strong influence of particle size which can be associated with the expression of B5 active sites. In the case of electride supported ruthenium is the nature of any structure sensitivity different?Hideo Hosono responded: Ru B5 sites exhibit high activity. I think this is also true for the electride support. The role of the electride is promotion of electrons to the N 2 absorbed on the Ru, leading to N2 dissociation. One thing to add: LaRuSi is a layered crystal. Ru atoms form a planar unit, with no B5 site, but this material works well. The turnover frequency (TOF) is 600 times higher than that of pure Ru powder. Density functional theory (DFT) calculations revealed that the dissociation of N2 occurs easily on the exposed Ru plane of LaRuSi. A systematic study provides rm evidence that layered Ru with a negative charge in LnRuSi is a new type of active site that differs signicantly from B5sites.1 I think the active site is not restricted to B5 sites.

AB - Justin S. J. Hargreaves opened discussion of the introductory lecture by Hideo Hosono: In the case of conventionally supported ruthenium catalysed ammonia synthesis there is a strong influence of particle size which can be associated with the expression of B5 active sites. In the case of electride supported ruthenium is the nature of any structure sensitivity different?Hideo Hosono responded: Ru B5 sites exhibit high activity. I think this is also true for the electride support. The role of the electride is promotion of electrons to the N 2 absorbed on the Ru, leading to N2 dissociation. One thing to add: LaRuSi is a layered crystal. Ru atoms form a planar unit, with no B5 site, but this material works well. The turnover frequency (TOF) is 600 times higher than that of pure Ru powder. Density functional theory (DFT) calculations revealed that the dissociation of N2 occurs easily on the exposed Ru plane of LaRuSi. A systematic study provides rm evidence that layered Ru with a negative charge in LnRuSi is a new type of active site that differs signicantly from B5sites.1 I think the active site is not restricted to B5 sites.

UR - http://www.scopus.com/inward/record.url?scp=85164329873&partnerID=8YFLogxK

U2 - 10.1039/d3fd90010j

DO - 10.1039/d3fd90010j

M3 - Comment / Debate

C2 - 37358417

AN - SCOPUS:85164329873

SN - 1359-6640

VL - 243

SP - 198

EP - 230

JO - Faraday Discussions

JF - Faraday Discussions

ER -

Heterogeneous catalytic and chemical looping routes to N2 activation: general discussion

Abstract

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Heterogeneous catalytic and chemical looping routes to N₂ activation: general discussion