The activity origin of FeCo Prussian blue analogue for ambient electrochemical hydrogenation of nitrate to ammonia in neutral electrolyte
Source abstract
Abstract
在温和的大气条件下通过电化学硝酸根还原反应(nitrate reduction reaction, NO3−RR)制氨是合成氨的可行方法, 也是一种很有前途的 储氢策略. 本研究首次将生长在碳纤维布上的铁钴普鲁士蓝类似物层 状立方阵列用作NO3−RR的电催化剂, 并且在中性的磷酸盐缓冲溶液中 获得了令人满意的氨产率(1788.4 µg h−1 cm−2)和法拉第效率(81.01%). 电化学结果和原位拉曼光谱表明, 氰基对提高催化活性至关重要. 通过 前沿轨道理论对催化剂的催化活性进行了解释: 氰基可以提高催化剂 最高占据态(即最高占据分子轨道)的能量, 促进电子从催化剂的最高 占据态跃迁至硝酸根离子的最低未占据分子轨道, 并实现吸附中间体 吉布斯自由能的优化, 从而加速NO3−RR.
Source: expertdata · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Hydrogen Storage and Materials · Advanced Photocatalysis Techniques
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (54)
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1. Liu C, Li Q, Wu C, et al. Single-boron catalysts for nitrogen reduction reaction. J Am Chem Soc, 2019, 141: 2884–288810.1021/jacs.8b13165 ↗
2. Jiao F, Xu B. Electrochemical ammonia synthesis and ammonia fuel cells. Adv Mater, 2019, 31: 180517310.1002/adma.201805173 ↗
3. Guo X, Gu J, Lin S, et al. Tackling the activity and selectivity challenges of electrocatalysts toward the nitrogen reduction reaction via atomically dispersed biatom catalysts. J Am Chem Soc, 2020, 142: 5709–572110.1021/jacs.9b13349 ↗
4. Yu B, Li H, White J, et al. Tuning the catalytic preference of ruthenium catalysts for nitrogen reduction by atomic dispersion. Adv Funct Mater, 2020, 30: 190566510.1002/adfm.201905665 ↗
5. Han X, Gerke CS, Banerjee S, et al. Strategic design of MoO2 nano-particles supported by carbon nanowires for enhanced electrocatalytic nitrogen reduction. ACS Energy Lett, 2020, 5: 3237–324310.1021/acsenergylett.0c01857 ↗
6. Gao R, Wang J, Huang ZF, et al. Pt/Fe2O3 with Pt-Fe pair sites as a catalyst for oxygen reduction with ultralow Pt loading. Nat Energy, 2021, 6: 614–62310.1038/s41560-021-00826-5 ↗
7. Li X, Zhang G, Shen P, et al. A defect engineered p-block SnS2-x catalyst for efficient electrocatalytic NO reduction to NH3. Inorg Chem Front, 2023, 10: 280–28710.1039/D2QI02118H ↗
8. Chen K, Zhang G, Li X, et al. Electrochemical NO reduction to NH3 on Cu single atom catalyst. Nano Res, 2023, 16: 5857–586310.1007/s12274-023-5384-9 ↗
9. Rosca V, Duca M, de Groot MT, et al. Nitrogen cycle electrocatalysis. Chem Rev, 2009, 109: 2209–224410.1021/cr8003696 ↗
10. Wang Y, Zhou W, Jia R, et al. Unveiling the activity origin of a copper-based electrocatalyst for selective nitrate reduction to ammonia. Angew Chem Int Ed, 2020, 59: 5350–535410.1002/anie.201915992 ↗
11. Wang M, Khan MA, Mohsin I, et al. Can sustainable ammonia synthesis pathways compete with fossil-fuel based Haber-Bosch processes?. Energy Environ Sci, 2021, 14: 2535–254810.1039/D0EE03808C ↗
12. van Langevelde PH, Katsounaros I, Koper MTM. Electrocatalytic nitrate reduction for sustainable ammonia production. Joule, 2021, 5: 290–29410.1016/j.joule.2020.12.025 ↗
13. Wang Z, Young SD, Goldsmith BR, et al. Increasing electrocatalytic nitrate reduction activity by controlling adsorption through PtRu alloying. J Catal, 2021, 395: 143–15410.1016/j.jcat.2020.12.031 ↗
14. Zhang X, Wang Y, Liu C, et al. Recent advances in non-noble metal electrocatalysts for nitrate reduction. Chem Eng J, 2021, 403: 12626910.1016/j.cej.2020.126269 ↗
15. Wang J, Feng T, Chen J, et al. Electrocatalytic nitrate/nitrite reduction to ammonia synthesis using metal nanocatalysts and bio-inspired metalloenzymes. Nano Energy, 2021, 86: 10608810.1016/j.nanoen.2021.106088 ↗
16. Glendening ED, Halpern AM. Ab initio calculations of nitrogen oxide reactions: Formation of N2O2, N2O3, N2O4, N2O5, and N4O2 from NO, NO2, NO3, and N2O. J Chem Phys, 2007, 127: 16430710.1063/1.2777145 ↗
17. Hirakawa H, Hashimoto M, Shiraishi Y, et al. Selective nitrate-to-ammonia transformation on surface defects of titanium dioxide photo-catalysts. ACS Catal, 2017, 7: 3713–372010.1021/acscatal.7b00611 ↗
18. Sun WJ, Ji HQ, Li LX, et al. Built-in electric field triggered interfacial accumulation effect for efficient nitrate removal at ultra-low concentration and electroreduction to ammonia. Angew Chem Int Ed, 2021, 60: 22933–2293910.1002/anie.202109785 ↗
19. Wang Y, Xu A, Wang Z, et al. Enhanced nitrate-to-ammonia activity on copper-nickel alloys via tuning of intermediate adsorption. J Am Chem Soc, 2020, 142: 5702–570810.1021/jacs.9b13347 ↗
20. Chen GF, Yuan Y, Jiang H, et al. Electrochemical reduction of nitrate to ammonia via direct eight-electron transfer using a copper-molecular solid catalyst. Nat Energy, 2020, 5: 605–61310.1038/s41560-020-0654-1 ↗
21. Xu Y, Wang M, Ren K, et al. Atomic defects in pothole-rich two-dimensional copper nanoplates triggering enhanced electrocatalytic selective nitrate-to-ammonia transformation. J Mater Chem A, 2021, 9: 16411–1641710.1039/D1TA04743D ↗
22. Fu X, Zhao X, Hu X, et al. Alternative route for electrochemical ammonia synthesis by reduction of nitrate on copper nanosheets. Appl Mater Today, 2020, 19: 10062010.1016/j.apmt.2020.100620 ↗
23. Zhu T, Chen Q, Liao P, et al. Single-atom Cu catalysts for enhanced electrocatalytic nitrate reduction with significant alleviation of nitrite production. Small, 2020, 16: 200452610.1002/smll.202004526 ↗
24. Qiu W, Chen X, Liu Y, et al. Confining intermediates within a catalytic nanoreactor facilitates nitrate-to-ammonia electrosynthesis. Appl Catal B-Environ, 2022, 315: 12154810.1016/j.apcatb.2022.121548 ↗
25. Cerrón-Calle GA, Fajardo AS, Sánchez-Sánchez CM, et al. Highly reactive Cu-Pt bimetallic 3D-electrocatalyst for selective nitrate reduction to ammonia. Appl Catal B-Environ, 2022, 302: 12084410.1016/j.apcatb.2021.120844 ↗
26. Gong Z, Zhong W, He Z, et al. Regulating surface oxygen species on copper (I) oxides via plasma treatment for effective reduction of nitrate to ammonia. Appl Catal B-Environ, 2022, 305: 12102110.1016/j.apcatb.2021.121021 ↗
27. Ye S, Chen Z, Zhang G, et al. Elucidating the activity, mechanism and application of selective electrosynthesis of ammonia from nitrate on cobalt phosphide. Energy Environ Sci, 2022, 15: 760–77010.1039/D1EE03097C ↗
28. Wang Y, Yu Y, Jia R, et al. Electrochemical synthesis of nitric acid from air and ammonia through waste utilization. Natl Sci Rev, 2019, 6: 730–73810.1093/nsr/nwz019 ↗
29. Deng X, Yang Y, Wang L, et al. Metallic Co nanoarray catalyzes selective NH3 production from electrochemical nitrate reduction at current densities exceeding 2 A cm−2. Adv Sci, 2021, 8: 200452310.1002/advs.202004523 ↗
30. Gao J, Jiang B, Ni C, et al. Non-precious Co3O4-TiO2/Ti cathode based electrocatalytic nitrate reduction: Preparation, performance and mechanism. Appl Catal B-Environ, 2019, 254: 391–40210.1016/j.apcatb.2019.05.016 ↗
31. Wu ZY, Karamad M, Yong X, et al. Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst. Nat Commun, 2021, 12: 287010.1038/s41467-021-23115-x ↗
32. Fang Z, Jin Z, Tang S, et al. Porous two-dimensional iron-cyano nanosheets for high-rate electrochemical nitrate reduction. ACS Nano, 2021, 16: 1072–108110.1021/acsnano.1c08814 ↗
33. Li P, Jin Z, Fang Z, et al. A single-site iron catalyst with preoccupied active centers that achieves selective ammonia electrosynthesis from nitrate. Energy Environ Sci, 2021, 14: 3522–353110.1039/D1EE00545F ↗
34. Jonoush ZA, Rezaee A, Ghaffarinejad A. Electrocatalytic nitrate reduction using Fe0/Fe3O4 nanoparticles immobilized on nickel foam: Selectivity and energy consumption studies. J Clean Prod, 2020, 242: 11856910.1016/j.jclepro.2019.118569 ↗
35. Lim J, Liu CY, Park J, et al. Structure sensitivity of Pd facets for enhanced electrochemical nitrate reduction to ammonia. ACS Catal, 2021, 11: 7568–757710.1021/acscatal.1c01413 ↗
36. Guo Y, Zhang R, Zhang S, et al. Pd doping-weakened intermediate adsorption to promote electrocatalytic nitrate reduction on TiO2 nanoarrays for ammonia production and energy supply with zinc-nitrate batteries. Energy Environ Sci, 2021, 14: 3938–394410.1039/D1EE00806D ↗
37. Jia R, Wang Y, Wang C, et al. Boosting selective nitrate electroreduction to ammonium by constructing oxygen vacancies in TiO2. ACS Catal, 2020, 10: 3533–354010.1021/acscatal.9b05260 ↗
38. Wang Z, Ortiz EM, Goldsmith BR, et al. Comparing electrocatalytic and thermocatalytic conversion of nitrate on platinum-ruthenium alloys. Catal Sci Technol, 2021, 11: 7098–710910.1039/D1CY01075A ↗
39. Li J, Zhan G, Yang J, et al. Efficient ammonia electrosynthesis from nitrate on strained ruthenium nanoclusters. J Am Chem Soc, 2020, 142: 7036–704610.1021/jacs.0c00418 ↗
40. Song X, Song S, Wang D, et al. Prussian blue analogs and their derived nanomaterials for electrochemical energy storage and electrocatalysis. Small Methods, 2021, 5: 200100010.1002/smtd.202001000 ↗
41. Wang J, Chen HM. Metallene pre-catalyst reconstruction for boosting catalytic performance. Chem Catal, 2022, 2: 3277–327910.1016/j.checat.2022.11.012 ↗
42. Xu YT, Peng Z, Han Y, et al. Insight into hydrogenation selectivity of the electrocatalytic nitrate-to-ammonia reduction reaction via enhancing the proton transport. ChemSusChem, 2022, 15: e20210245010.1002/cssc.202102450 ↗
43. McEnaney JM, Blair SJ, Nielander AC, et al. Electrolyte engineering for efficient electrochemical nitrate reduction to ammonia on a titanium electrode. ACS Sustain Chem Eng, 2020, 8: 2672–268110.1021/acssuschemeng.9b05983 ↗
44. Kang L, Ren H, Xing Z, et al. Hierarchical porous CoxFe3−xO4 nano-cubes obtained by calcining Prussian blue analogues as anodes for lithium-ion batteries. New J Chem, 2020, 44: 12546–1255510.1039/D0NJ01027H ↗
45. Wang Q, He S, Wang N, et al. Synthesis of CoFe Prussian blue analogue/carbon nanotube composite material and its application in the catalytic epoxidation of styrene. New J Chem, 2016, 40: 3244–325110.1039/C5NJ03618F ↗
46. Ye S, Zhang Y, Xiong W, et al. Construction of tetrahedral CoO4 vacancies for activating the high oxygen evolution activity of Co3-xO4-δ porous nanosheet arrays. Nanoscale, 2020, 12: 11079–1108710.1039/D0NR00744G ↗
47. Wang X, Ouyang T, Wang L, et al. Redox-inert Fe3+ ions in octahedral sites of Co-Fe spinel oxides with enhanced oxygen catalytic activity for rechargeable zinc-air batteries. Angew Chem, 2019, 131: 13425–1343010.1002/ange.201907595 ↗
48. Samain L, Gilbert B, Grandjean F, et al. Redox reactions in Prussian blue containing paint layers as a result of light exposure. J Anal At Spectrom, 2013, 28: 524–53510.1039/c3ja30359d ↗
49. Hsu SH, Hung SF, Wang HY, et al. Tuning the electronic spin state of catalysts by strain control for highly efficient water electrolysis. Small Methods, 2018, 2: 180000110.1002/smtd.201800001 ↗
50. Garcia-Segura S, Lanzarini-Lopes M, Hristovski K, et al. Electrocatalytic reduction of nitrate: Fundamentals to full-scale water treatment applications. Appl Catal B-Environ, 2018, 236: 546–56810.1016/j.apcatb.2018.05.041 ↗
51. Wang Y, Zhang L, Niu Y, et al. Boosting NH3 production from nitrate electroreduction via electronic structure engineering of Fe3C nano-flakes. Green Chem, 2021, 23: 7594–760810.1039/D1GC01913A ↗
52. Miessler G, Tarr D. Inorganic Chemistry. 3rd ed. New York: Pearson Education. 154–156
53. Beagan DM, Cabelof AC, Caulton KG. Back donation, intramolecular electron transfer and N–O bond scission targeting nitrogen oxyanion reduction: how can a metal complex assist? Dalton Trans, 2021, 50: 2149–215710.1039/D0DT03430D ↗
54. Butcher Jr. DP, Gewirth AA. Nitrate reduction pathways on Cu single crystal surfaces: Effect of oxide and Cl−. Nano Energy, 2016, 29: 457–46510.1016/j.nanoen.2016.06.024 ↗