journal article·2020-11-13Open access

Mechanocatalytic Ammonia Synthesis over TiN in Transient Microenvironments

Andrew W. Tricker, Karoline L. Hebisch, Marco Buchmann, Yu-Hsuan Liu, Marcus Rose, Eli Stavitski, Andrew J. Medford, Marta C. Hatzell, Carsten Sievers

ACS Energy Letters· Volume 5· Issue 11

Abstract

Environmentally friendly and energy-efficient ways to produce ammonia are essential to meet global food demands. Here, a new approach for ammonia production at nominally ambient conditions is introduced. As proof of concept, ammonia is synthesized mechanocatalytically by ball milling titanium in a continuous gas flow. The ammonia synthesis reaction is proposed to follow a transient Mars–van Krevelen mechanism under mechanically activated conditions, where molecular nitrogen incorporation into the titanium lattice and titanium nitride hydrogenation occur in thermodynamically distinct environments. X-ray powder diffraction and X-ray absorption spectroscopy confirm the formation of titanium nitride from titanium and N2. The reactivity of nitrided titanium supports that lattice nitrogen plays a role in ammonia formation. The in situ formed titanium nitride is catalytically active, and the nitride regeneration reaction is determined to be the rate-limiting step. A preliminary technoeconomic analysis shows that this approach could be feasible for distributed ammonia production.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Nanomaterials for catalytic reactions · Hydrogen Storage and Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States

Renewable Bioproducts Institute, Georgia Institute of Technology, Atlanta, Georgia 30332, United States

Department of Chemistry, Technical University of Darmstadt, 64287 Darmstadt, Germany

School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States

National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, United States

The George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States

Funding

Bundesministerium f?r Bildung und Forschung · BASF · Deutsche Forschungsgemeinschaft · Division of Electrical, Communications and Cyber Systems · Division of Chemical, Bioengineering, Environmental, and Transport Systems

References (57)

Show source-provided references
1. 10.1038/2267210.1038/22672 ↗
2. 10.1038/ngeo32510.1038/ngeo325 ↗
3. 10.1002/14356007.a02_143.pub210.1002/14356007.a02_143.pub2 ↗
4. 10.1016/j.jdeveco.2017.02.00710.1016/j.jdeveco.2017.02.007 ↗
5. 10.1021/acscatal.7b0043910.1021/acscatal.7b00439 ↗
6. 10.1021/acsenergylett.8b0219710.1021/acsenergylett.8b02197 ↗
7. 10.1016/j.joule.2019.05.00110.1016/j.joule.2019.05.001 ↗
8. 10.1016/j.joule.2017.07.00810.1016/j.joule.2017.07.008 ↗
9. 10.1016/j.joule.2018.04.01410.1016/j.joule.2018.04.014 ↗
10. 10.1021/acsenergylett.8b0048710.1021/acsenergylett.8b00487 ↗
11. 10.1021/ja00464a01510.1021/ja00464a015 ↗
12. 10.1021/jacs.8b0846410.1021/jacs.8b08464 ↗
13. 10.1039/C8FD00191J10.1039/C8FD00191J ↗
14. 10.1038/s41929-018-0045-110.1038/s41929-018-0045-1 ↗
15. 10.1021/acsenergylett.9b0026310.1021/acsenergylett.9b00263 ↗
16. 10.1039/C5SC00789E10.1039/C5SC00789E ↗
17. 10.1016/j.apcatb.2017.04.07310.1016/j.apcatb.2017.04.073 ↗
18. 10.1021/acsenergylett.9b0086010.1021/acsenergylett.9b00860 ↗
19. 10.1039/C1CS15171A10.1039/C1CS15171A ↗
20. 10.1002/anie.20190675510.1002/anie.201906755 ↗
21. 10.1016/j.tetlet.2015.03.13510.1016/j.tetlet.2015.03.135 ↗
22. 10.1021/acs.jpclett.5b0183710.1021/acs.jpclett.5b01837 ↗
23. 10.1021/ja904256510.1021/ja9042565 ↗
24. 10.1002/anie.20181090210.1002/anie.201810902 ↗
25. 10.1021/jacs.9b0441310.1021/jacs.9b04413 ↗
26. 10.1002/cssc.20110077010.1002/cssc.201100770 ↗
27. 10.1039/C2GC36456E10.1039/C2GC36456E ↗
28. 10.1016/j.cattod.2017.04.06610.1016/j.cattod.2017.04.066 ↗
29. 10.1039/c2cs35442j10.1039/c2cs35442j ↗
30. 10.1016/j.cej.2019.12295410.1016/j.cej.2019.122954 ↗
31. 10.1016/S0079-6425(99)00010-910.1016/S0079-6425(99)00010-9 ↗
32. 10.1002/anie.20130599210.1002/anie.201305992 ↗
33. 10.1007/s10853-017-1153-z10.1007/s10853-017-1153-z ↗
34. 10.1063/1.10628510.1063/1.106285 ↗
35. 10.2320/matertrans1989.34.121210.2320/matertrans1989.34.1212 ↗
36. 10.1126/sciadv.aax827510.1126/sciadv.aax8275 ↗
37. 10.1002/zaac.1961312030610.1002/zaac.19613120306 ↗
38. 10.1002/zfch.1974014023010.1002/zfch.19740140230 ↗
39. 10.1063/1.33656310.1063/1.336563 ↗
40. 10.1007/BF0264771210.1007/BF02647712 ↗
41. 10.1007/BF0278240910.1007/BF02782409 ↗
42. 10.1007/s13203-014-0049-y10.1007/s13203-014-0049-y ↗
43. 10.1021/acscatal.5b0191810.1021/acscatal.5b01918 ↗
44. 10.1021/acscatal.9b0160610.1021/acscatal.9b01606 ↗
45. 10.1063/1.11908410.1063/1.119084 ↗
46. 10.1557/JMR.2002.024410.1557/JMR.2002.0244 ↗
47. 10.1007/s10853-017-1734-x10.1007/s10853-017-1734-x ↗
48. 10.1021/acscatal.8b0212010.1021/acscatal.8b02120 ↗
49. 10.1038/s41586-019-1260-x10.1038/s41586-019-1260-x ↗
50. 10.1021/acsenergylett.9b0228610.1021/acsenergylett.9b02286 ↗
51. 10.1021/j100411a03110.1021/j100411a031 ↗
52. 10.1016/j.jssc.2007.12.00110.1016/j.jssc.2007.12.001 ↗
53. 10.1021/ja010963d10.1021/ja010963d ↗
54. Michaud D. · 2017 · 2020
55. 10.1021/acscatal.6b0042810.1021/acscatal.6b00428 ↗
56. 10.1002/cctc.20180143810.1002/cctc.201801438 ↗
57. 10.1080/0161494090304866110.1080/01614940903048661 ↗