Evaluation of Pt-Rh Nanoparticle-Based Electrodes for the Electrochemical Reduction of Nitrogen to Ammonia

被引:6
作者
Amrine, Roumayssa [1 ]
Montiel, Miguel A. [1 ]
Montiel, Vicente [1 ]
Solla-Gullon, Jose [1 ]
机构
[1] Univ Alicante, Inst Electrochem, Apdo 99, Alicante 03080, Spain
关键词
Electrocatalysis; Nitrogen reduction; Ammonia; Pt-Rh; Nanoparticles;
D O I
10.1007/s12678-024-00870-1
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Ammonia (NH3) is one of the most used chemicals. Industrially, ammonia is produced by hydrogenation of N-2 through the Haber-Bosch process, a process in which enormous amounts of CO2 are released and requires a huge energy consumption (similar to 2% of the total global energy). Therefore, it is of paramount importance to explore more sustainable and environmentally friendly routes to produce NH3. The electrochemical nitrogen reduction reaction (NRR) to ammonia represents a promising alternative that is receiving great attention but still needs to be significantly improved to be economically competitive. In this work, the NRR is studied on Pt-Rh nanoparticle-based electrodes. Carbon-supported Pt-Rh nanoparticles (2-4 nm) with different Pt:Rh atomic compositions were synthesized and subsequently airbrushed onto carbon Toray paper to fabricate electrodes. The electrochemical NRR experiments were performed in a H-cell in 0.1 M Na2SO4 solution. The results obtained show interesting faradaic efficiencies (FE) towards NH3 which range between 5 and 23% and reasonable and reliable NH3 yield values of about 4.5 mu g h(-1) mg(cat)(-1), depending on the atomic composition of the electrocatalysts and the metal loading. The electrodes also showed good stability and recyclability (constant FE and NH3 yield in five consecutive experiments).
引用
收藏
页码:239 / 250
页数:12
相关论文
共 70 条
[1]   A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements [J].
Andersen, Suzanne Z. ;
Colic, Viktor ;
Yang, Sungeun ;
Schwalbe, Jay A. ;
Nielander, Adam C. ;
McEnaney, Joshua M. ;
Enemark-Rasmussen, Kasper ;
Baker, Jon G. ;
Singh, Aayush R. ;
Rohr, Brian A. ;
Statt, Michael J. ;
Blair, Sarah J. ;
Mezzavilla, Stefano ;
Kibsgaard, Jakob ;
Vesborg, Peter C. K. ;
Cargnello, Matteo ;
Bent, Stacey F. ;
Jaramillo, Thomas F. ;
Stephens, Ifan E. L. ;
Norskov, Jens K. ;
Chorkendorff, Ib .
NATURE, 2019, 570 (7762) :504-+
[2]   Electrochemical Reduction of N2 under Ambient Conditions for Artificial N2 Fixation and Renewable Energy Storage Using N2/NH3 Cycle [J].
Bao, Di ;
Zhang, Qi ;
Meng, Fan-Lu ;
Zhong, Hai-Xia ;
Shi, Miao-Miao ;
Zhang, Yu ;
Yan, Jun-Min ;
Jiang, Qing ;
Zhang, Xin-Bo .
ADVANCED MATERIALS, 2017, 29 (03)
[3]   THE SOLUBILITY OF NITROGEN AND AIR IN LIQUIDS [J].
BATTINO, R ;
RETTICH, TR ;
TOMINAGA, T .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1984, 13 (02) :563-600
[4]   Mechanism of molybdenum nitrogenase [J].
Burgess, BK ;
Lowe, DJ .
CHEMICAL REVIEWS, 1996, 96 (07) :2983-3011
[5]   Beyond fossil fuel-driven nitrogen transformations [J].
Chen, Jingguang G. ;
Crooks, Richard M. ;
Seefeldt, Lance C. ;
Bren, Kara L. ;
Bullock, R. Morris ;
Darensbourg, Marcetta Y. ;
Holland, Patrick L. ;
Hoffman, Brian ;
Janik, Michael J. ;
Jones, Anne K. ;
Kanatzidis, Mercouri G. ;
King, Paul ;
Lancaster, Kyle M. ;
Lymar, Sergei V. ;
Pfromm, Peter ;
Schneider, William F. ;
Schrock, Richard R. .
SCIENCE, 2018, 360 (6391)
[6]   Identification and elimination of false positives in electrochemical nitrogen reduction studies [J].
Choi, Jaecheol ;
Suryanto, Bryan H. R. ;
Wang, Dabin ;
Du, Hoang-Long ;
Hodgetts, Rebecca Y. ;
Vallana, Federico M. Ferrero ;
MacFarlane, Douglas R. ;
Simonov, Alexandr N. .
NATURE COMMUNICATIONS, 2020, 11 (01)
[7]   Rhodium-molybdenum oxide electrocatalyst with dual active sites for electrochemical ammonia synthesis under neutral pH condition [J].
Chung, Sunki ;
Seo, Dong Han ;
Choi, Minjun ;
Mao, Xin ;
Du, Aijun ;
Ham, Kahyun ;
Giddey, Sarbjit ;
Lee, Jaeyoung ;
Ju, HyungKuk .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2021, 896 (896)
[8]   A Review of Electrocatalytic Reduction of Dinitrogen to Ammonia under Ambient Conditions [J].
Cui, Xiaoyang ;
Tang, Cheng ;
Zhang, Qiang .
ADVANCED ENERGY MATERIALS, 2018, 8 (22)
[9]   High activity of Pt-Rh supported on C-ITO for ethanol oxidation in alkaline medium [J].
de Carmargo, V. F. ;
Fontes, E. H. ;
Nandenha, J. ;
de Souza, R. F. B. ;
Neto, A. O. .
RESEARCH ON CHEMICAL INTERMEDIATES, 2020, 46 (02) :1555-1570
[10]   The rational adjusting of proton-feeding by Pt-doped FeP/C hollow nanorod for promoting nitrogen reduction kinetics [J].
Deng, Ying ;
Xiao, Zhenyu ;
Wang, Zuochao ;
Lai, Jianping ;
Liu, Xiaobin ;
Zhang, Dan ;
Han, Yi ;
Li, Shaoxiang ;
Sun, Wei ;
Wang, Lei .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2021, 291