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Vol. 16 (2024)

Highly Sensitive Ammonia Gas Sensors at Room Temperature Based on the Catalytic Mechanism of N, C Coordinated Ni Single-Atom Active Center

https://doi.org/10.1007/s40820-024-01484-4
Wenjing Quan
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Jia Shi
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Min Zeng
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Wen Lv
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Xiyu Chen
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Chao Fan
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Yongwei Zhang
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Zhou Liu
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Xiaolu Huang
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Jianhua Yang
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Nantao Hu
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Tao Wang
Shanghai Key Laboratory of Intelligent Sensing and Detection Technology, School of Mechanical and Power Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Zhi Yang
National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China

Corresponding Author: Zhi Yang

zhiyang@sjtu.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 277

Abstract

Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia (NH3). In this study, we propose to exploit single-atom catalytic activation and targeted adsorption properties to achieve highly sensitive and selective NH3 gas detection. Specifically, Ni single-atom active sites based on N, C coordination (Ni–N–C) were interfacially confined on the surface of two-dimensional (2D) MXene nanosheets (Ni–N–C/Ti3C2Tx), and a fully flexible gas sensor (MNPE–Ni–N–C/Ti3C2Tx) was integrated. The sensor demonstrates a remarkable response value to 5 ppm NH3 (27.3%), excellent selectivity for NH3, and a low theoretical detection limit of 12.1 ppb. Simulation analysis by density functional calculation reveals that the Ni single-atom center with N, C coordination exhibits specific targeted adsorption properties for NH3. Additionally, its catalytic activation effect effectively reduces the Gibbs free energy of the sensing elemental reaction, while its electronic structure promotes the spill-over effect of reactive oxygen species at the gas–solid interface. The sensor has a dual-channel sensing mechanism of both chemical and electronic sensitization, which facilitates efficient electron transfer to the 2D MXene conductive network, resulting in the formation of the NH3 gas molecule sensing signal. Furthermore, the passivation of MXene edge defects by a conjugated hydrogen bond network enhances the long-term stability of MXene-based electrodes under high humidity conditions. This work achieves highly sensitive room-temperature NH3 gas detection based on the catalytic mechanism of Ni single-atom active center with N, C coordination, which provides a novel gas sensing mechanism for room-temperature trace gas detection research.


Highlights:
1 Exploiting single-atom catalytic activation and targeted adsorption properties, Ni single-atom active sites based on N, C coordination are constructed on the surface of two-dimensional MXene nanosheets (Ni–N–C/Ti3C2Tx), enabling highly sensitive and selective NH3 gas detection.
2 The catalytic activation effect of Ni–N–C/Ti3C2Tx effectively reduces the Gibbs free energy of the sensing elemental reaction, while its electronic structure promotes the spill-over effect of reactive oxygen species at the gas–solid interface.
3 An end-sealing passivation strategy utilizing a conjugated hydrogen bond network of the conductive polymer was employed on MXene-based flexible electrodes, effectively mitigating the oxidative degradation of MXene-based gas sensors.

Keywords

Gas sensor Single atom Catalytic activation Targeted adsorption End-sealing passivation
Quan, Wenjing, Jia Shi, Min Zeng, Wen Lv, Xiyu Chen, Chao Fan, Yongwei Zhang, Zhou Liu, Xiaolu Huang, Jianhua Yang, Nantao Hu, Tao Wang, and Zhi Yang. 2024. “Highly Sensitive Ammonia Gas Sensors at Room Temperature Based on the Catalytic Mechanism of N, C Coordinated Ni Single-Atom Active Center”. Nano-Micro Letters 16 (August):277. https://doi.org/10.1007/s40820-024-01484-4.
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References
  1. Y.J. Su, G.R. Chen, C.X. Chen, Q.C. Gong, G.Z. Xie et al., Self-powered respiration monitoring enabled by a triboelectric nanogenerator. Adv. Mater. 33(35), 2101262 (2021). https://doi.org/10.1002/adma.202101262
  2. G. Peng, U. Tisch, O. Adams, M. Hakim, N. Shehada et al., Diagnosing lung cancer in exhaled breath using gold nanops. Nat. Nanotechnol. 4(10), 669–673 (2009). https://doi.org/10.1038/nnano.2009.235
  3. T. Wang, Y. Wu, Y. Zhang, W. Lv, X. Chen et al., Portable electronic nose system with elastic architecture and fault tolerance based on edge computing, ensemble learning, and sensor swarm. Sens. Actuators B: Chem. 375, 132925 (2023). https://doi.org/10.1016/j.snb.2022.132925
  4. C. Jackson, G.T. Smith, D.W. Inwood, A.S. Leach, P.S. Whalley et al., Electronic metal-support interaction enhanced oxygen reduction activity and stability of boron carbide supported platinum. Nat. Commun. 8, 15802 (2017). https://doi.org/10.1038/ncomms15802
  5. S.Y. Jeong, Y.K. Moon, J. Wang, J.H. Lee, Exclusive detection of volatile aromatic hydrocarbons using bilayer oxide chemiresistors with catalytic overlayers. Nat. Commun. 14(1), 233 (2023). https://doi.org/10.1038/s41467-023-35916-3
  6. T.S. Chu, C. Rong, L. Zhou, X.Y. Mao, B.W. Zhang et al., Progress and perspectives of single-atom catalysts for gas sensing. Adv. Mater. 35, 2206783 (2022). https://doi.org/10.1002/adma.202206783
  7. L.J. Zhang, N. Jin, Y.B. Yang, X.Y. Miao, H. Wang et al., Advances on axial coordination design of single-atom catalysts for energy electrocatalysis: a review. Nano-Micro Lett. 15(1), 228 (2023). https://doi.org/10.1007/s40820-023-01196-1
  8. A.A. Peyghan, S.F. Rastegar, N.L. Hadipour, DFT study of NH3 adsorption on pristine, Ni- and Si-doped graphynes. Phys. Lett. A 378(30–31), 2184–2190 (2014). https://doi.org/10.1016/j.physleta.2014.05.016
  9. C.F. Yang, R. Zhao, H. Xiang, J. Wu, W.D. Zhong et al., Ni-activated transition metal carbides for efficient hydrogen evolution in acidic and alkaline solutions. Adv. Energy Mater. 10(37), 2002260 (2020). https://doi.org/10.1002/aenm.202002260
  10. M. Zhou, Y. Jiang, G. Wang, W.J. Wu, W.X. Chen et al., Single-atom Ni–N4 provides a robust cellular NO sensor. Nat. Commun. 11(1), 3188 (2020). https://doi.org/10.1038/s41467-020-17018-6
  11. H. Shin, W.G. Jung, D.H. Kim, J.S. Jang, Y.H. Kim et al., Single-atom Pt stabilized on one-dimensional nanostructure support via carbon nitride/SnO2 heterojunction trapping. ACS Nano 14(9), 11394–11405 (2020). https://doi.org/10.1021/acsnano.0c03687
  12. H. Xu, Y.T. Zhao, Q. Wang, G.Y. He, H.Q. Chen, Supports promote single-atom catalysts toward advanced electrocatalysis. Coord. Chem. Rev. 451, 214261 (2022). https://doi.org/10.1016/j.ccr.2021.214261
  13. Z.J. Yang, S.Y. Lv, Y.Y. Zhang, J. Wang, L. Jiang et al., Self-assembly 3D porous crumpled MXene spheres as efficient gas and pressure sensing material for transient all–MXene sensors. Nano-Micro Lett. 14(1), 56 (2022). https://doi.org/10.1007/s40820-022-00796-7
  14. M. Khazaei, A. Ranjbar, M. Ghorbani-Asl, M. Arai, T. Sasaki et al., Nearly free electron states in MXenes. Phys. Rev. B 93, 205125 (2016). https://doi.org/10.1103/PhysRevB.93.205125
  15. R.X. Hu, D.W. Sha, X. Cao, C.J. Lu, Y.C. Wei et al., Anchoring metal-organic framework-derived ZnTe@C onto elastic Ti3C2Tx MXene with 0D/2D dual confinement for ultrastable potassium-ion storage. Adv. Energy Mater. 12(47), 2203118 (2022). https://doi.org/10.1002/aenm.202203118
  16. S.J. Kim, H.J. Koh, C.E. Ren, O. Kwon, K. Maleski et al., Metallic Ti3C2Tx MXene gas sensors with ultrahigh signal-to-noise ratio. ACS Nano 12(2), 986–993 (2018). https://doi.org/10.1021/acsnano.7b07460
  17. W.J. Quan, J. Shi, H.Y. Luo, C. Fan, W. Lv et al., Fully flexible MXene-based gas sensor on paper for highly sensitive room-temperature nitrogen dioxide detection. ACS Sens. 8(1), 103–113 (2023). https://doi.org/10.1021/acssensors.2c01748
  18. F.C. Cao, Y. Zhang, H.Q. Wang, K. Khan, A.K. Tareen et al., Recent advances in oxidation stable chemistry of 2D MXenes. Adv. Mater. 34, 2107554 (2022). https://doi.org/10.1002/adma.202107554
  19. X.F. Zhao, A. Vashisth, E. Prehn, W.M. Sun, S. Shah et al., Antioxidants unlock shelf-stable Ti3C2Tx (MXene) nanosheet dispersions. Matter 1(2), 513–526 (2019). https://doi.org/10.1016/j.matt.2019.05.020
  20. W.Y. Chen, S.N. Lai, C.C. Yen, X.F. Jiang, D. Peroulis et al., Surface functionalization of Ti3C2Tx MXene with highly reliable superhydrophobic protection for volatile organic compounds sensing. ACS Nano 14(9), 11490–11501 (2020). https://doi.org/10.1021/acsnano.0c03896
  21. J.T. Lee, B.C. Wyatt, G.A. Davis Jr., A.N. Masterson, A.L. Pagan et al., Covalent surface modification of Ti3C2Tx MXene with chemically active polymeric ligands producing highly conductive and ordered microstructure films. ACS Nano 15(12), 19600–19612 (2021). https://doi.org/10.1021/acsnano.1c06670
  22. G.F. He, F.G. Ning, X. Liu, Y.X. Meng, Z.W. Lei et al., High-performance and long-term stability of MXene/PEDOT:PSS-decorated cotton yarn for wearable electronics applications. Adv. Fiber Mater. 6, 1–20 (2023). https://doi.org/10.1007/s42765-023-00348-7
  23. G. Kresse, J. Furthmuller, Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Comput. Mater. Sci. 6(1), 15–50 (1996). https://doi.org/10.1016/0927-0256(96)00008-0
  24. G. Kresse, J. Furthmuller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54(16), 11169–11186 (1996). https://doi.org/10.1103/PhysRevB.54.11169
  25. G. Henkelman, A. Arnaldsson, H. Jonsson, A fast and robust algorithm for Bader decomposition of charge density. Comput. Mater. Sci. 36(3), 354–360 (2006). https://doi.org/10.1016/j.commatsci.2005.04.010
  26. J.X. Li, Y.L. Du, C.X. Huo, S. Wang, C. Cui, Thermal stability of two-dimensional Ti2C nanosheets. Ceram. Int. 41(2), 2631–2635 (2015). https://doi.org/10.1016/j.ceramint.2014.10.070
  27. M.Q. Zhao, X.Q. Xie, C.E. Ren, T. Makaryan, B. Anasori et al., Hollow MXene spheres and 3D macroporous MXene frameworks for Na-ion storage. Adv. Mater. 29(37), 1702410 (2017). https://doi.org/10.1002/adma.201702410
  28. L.Y. Zhu, X.Y. Miao, L.X. Ou, L.W. Mao, K.P. Yuan et al., Heterostructured α-Fe2O3@ZnO@ZIF-8 core-shell nanowires for a highly selective MEMS-based ppb-level H2S gas sensor system. Small 18, 2204828 (2022). https://doi.org/10.1002/smll.202204828
  29. X.X. Wang, D.A. Cullen, Y.T. Pan, S. Hwang, M. Wang et al., Nitrogen–Coordinated single cobalt atom catalysts for oxygen reduction in proton exchange membrane fuel cells. Adv. Mater. 30, 1706758 (2018). https://doi.org/10.1002/adma.201706758
  30. X. Zhang, H. Su, P.X. Cui, Y.Y. Cao, Z.Y. Teng et al., Developing Ni single-atom sites in carbon nitride for efficient photocatalytic H2O2 production. Nat. Commun. 14, 7115 (2023). https://doi.org/10.1038/s41467-023-42887-y
  31. H.F. Xiong, A.K. Datye, Y. Wang, Thermally stable single-atom heterogeneous catalysts. Adv. Mater. 33(50), 2004319 (2021). https://doi.org/10.1002/adma.202004319
  32. S. Uzun, M. Schelling, K. Hantanasirisakul, T.S. Mathis, R. Askeland et al., Additive-free aqueous MXene inks for thermal inkjet printing on textiles. Small 17(1), 2006376 (2021). https://doi.org/10.1002/smll.202006376
  33. J.X. Ma, S.H. Zheng, Y.X. Cao, Y.Y. Zhu, P. Das et al., Aqueous MXene/PH1000 hybrid inks for inkjet-printing micro-supercapacitors with unprecedented volumetric capacitance and modular self-powered microelectronics. Adv. Energy Mater. 11(23), 2100746 (2021). https://doi.org/10.1002/aenm.202100746
  34. C.F. Zhang, L. McKeon, M.P. Kremer, S.H. Park, O. Ronan et al., Additive-free MXene inks and direct printing of micro-supercapacitors. Nat. Commun. 10, 1795 (2019). https://doi.org/10.1038/s41467-019-09398-1
  35. J. Liu, L. Mckeon, J. Garcia, S. Pinilla, S. Barwich et al., Additive manufacturing of Ti3C2–MXene-functionalized conductive polymer hydrogels for electromagnetic-interference shielding. Adv. Mater. 34(5), 2106253 (2022). https://doi.org/10.1002/adma.202106253
  36. J. Jang, H. Kang, H.C.N. Chakravarthula, V. Subramanian, Fully inkjet-printed transparent oxide thin film transistors using a fugitive wettability switch. Adv. Electron. Mater. 1(7), 1500086 (2015). https://doi.org/10.1002/aelm.201500086
  37. I. Caballero-Quintana, J.L. Maldonado, M.A. Meneses-Nava, O. Barbosa-Garcia, J. Valenzuela-Benavides et al., Semiconducting polymer thin films used in organic solar cells: a scanning tunneling microscopy study. Adv. Electron. Mater. 5(2), 1800499 (2019). https://doi.org/10.1002/aelm.201800499
  38. O. Bubnova, Z.U. Khan, A. Malti, S. Braun, M. Fahlman et al., Optimization of the thermoelectric figure of merit in the conducting polymer poly(3,4-ethylenedioxythiophene). Nat. Mater. 10(6), 429–433 (2011). https://doi.org/10.1038/nmat3012
  39. Y.Z. Shao, L.S. Wei, X.Y. Wu, C.M. Jiang, Y. Yao et al., Room-temperature high-precision printing of flexible wireless electronics based on MXene inks. Nat. Commun. 13(1), 3223 (2022). https://doi.org/10.1038/s41467-022-30648-2
  40. X.Y. Chen, L.W. Kong, J.A.A. Mehrez, C. Fan, W.J. Quan et al., Outstanding humidity chemiresistors based on imine-linked covalent organic framework films for human respiration monitoring. Nano-Micro Lett. 15(1), 149 (2023). https://doi.org/10.1007/s40820-023-01107-4
  41. X.T. Jiang, A.V. Kuklin, A. Baev, Y.Q. Ge, H. Agren et al., Two-dimensional MXenes: from morphological to optical, electric, and magnetic properties and applications. Phys. Rep. 848, 1–58 (2020). https://doi.org/10.1016/j.physrep.2019.12.006
  42. G.P. Neupane, B.W. Wang, M. Tebyetekerwa, H.T. Nguyen, M. Taheri et al., Highly enhanced light-matter interaction in MXene quantum dots-monolayer WS2 heterostructure. Small 17(11), 2006309 (2021). https://doi.org/10.1002/smll.202006309
  43. T. Cheng, Y.Z. Zhang, S. Wang, Y.L. Chen, S.Y. Gao et al., Conductive hydrogel-based electrodes and electrolytes for stretchable and self-healable supercapacitors. Adv. Funct. Mater. 31(24), 2101303 (2021). https://doi.org/10.1002/adfm.202101303
  44. J. Li, J. Cao, B. Lu, G.Y. Gu, 3D-printed PEDOT:PSS for soft robotics. Nat. Rev. Mater. 8(9), 604–622 (2023). https://doi.org/10.1038/s41578-023-00587-5
  45. J.M. Luo, C.L. Wang, H. Wang, X.F. Hu, E. Matios et al., Pillared MXene with ultralarge interlayer spacing as a stable matrix for high performance sodium metal anodes. Adv. Funct. Mater. 29(3), 1805946 (2019). https://doi.org/10.1002/adfm.201805946
  46. Q.X. Feng, B.Y. Huang, X.G. Li, Graphene-based heterostructure composite sensing materials for detection of nitrogen-containing harmful gases. Adv. Funct. Mater. 31(41), 2104058 (2021). https://doi.org/10.1002/adfm.202104058
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