Recent Progress of Electric Conductive Metal-Organic Frameworks Thin Film

doi:10.6023/A22010024

Abstract

Electric conductive metal-organic frameworks (EC-MOFs) are a family of novel solid conductive materials with both conductivity and porosity. They have a wide of researches in the field of electricity, such as fuel cells, electrocatalysis, supercapacitors, thermoelectrics and sensors. Since the EC-MOFs are difficult to process into a film, which hinders their further development in electronic devices, so, the research on EC-MOFs film and their electrical properties have attracted much attention in recent years. In this review, the latest research progress of EC-MOFs film is summarized including the preparation methods of EC-MOFs film and their applications in the field of electricity. Finally, the opportunities and challenges of future development for EC-MOFs film are briefly presented.

Key words: electric conductive metal-organic frameworks, thin film preparation, electrical applications

Cite this article

Linan Cao, Min Wei. Recent Progress of Electric Conductive Metal-Organic Frameworks Thin Film[J]. Acta Chimica Sinica, 2022, 80(7): 1042-1056.

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Fig. & Tab. 19

Figure 1. Preparation methods and application fields of EC-MOFs thin films in this review

Figure 2. Timeline of important events in EC-MOFs thin film preparation

Figure 3. (a) Schematic diagram of the layer-by-layer self-assembly liquid phase epitaxy spray method to fabricate Cu3(HHTP)2 thin films, adapted from the literature [44]; (b) schematic diagram of the layer-by-layer self-assembled liquid phase epitaxy immersion method to fabricate Cu3(HHTP)2 thin films, adapted from the literature [46]; (c) schematic diagram of layer-by-layer self-assembled liquid phase epitaxy immersion method to fabricate Cu3(HHTP)2 thin films on 3D substrates, adapted from the literature [48]

Figure 4. (a) Schematic diagram of the liquid-liquid interfacial method to fabricate Cu-CAT thin films, (b) photograph of the Cu-CAT film formed at the interface between organic solution and aqueous solution, adapted from the literature [54]; Formation of the Ag3BHT2 thin film by liquid-liquid interfacial method, (c) beginning of the reaction, (d) the formation of the thin film, adapted from the literature [55]

Figure 5. (a) Schematic diagram of the gas-liquid interfacial method to fabricate Ni3(HITP)2 thin films, adapted from the literature [59]; (b) schematic diagram of the gas-liquid interfacial method to fabricate Cu2[PcM-O8] thin films, adapted from the literature [61]

Figure 6. (a) Schematic diagram of the steam assisted conversion method to fabricate NiPc-CoTAA thin films, adapted from the literature [66]; (b) schematic diagram of the steam assisted conversion method to fabricate Ni3(HITP)2 thin films, adapted from the literature [67]

Figure 7. (a) Schematic diagram of the electrochemical process to fabricate Cu3(HHTP)2 thin films, adapted from the literature [70]; (b) schematic diagram of the Face-to-Face confinement method to fabricate EC-MOF thin films, adapted from the literature [71]

Figure 8. SEM of Cu3(HHTP)2 thin film prepared via LbL method on (a) 2D substrate, adapted from the literature [44]; (b) 3D substrate, adapted from the literature [48]; (c) HR-TEM of Cu3(HHTP)2 thin film prepared by liquid-liquid interface method, adapted from the literature [54]; (d) SEM of Cu3(HHTP)2 thin film prepared by electrochemical method, adapted from the literature [70]

Figure 9. (a) The response-recovery curve of Cu3(HHTP)2 thin films toward NH3 with different concentrations; (b) the column chart of responses toward different VOCs of Cu3(HHTP)2, adapted from the literature [44]; (c) a response comparison of Cu-HHTP-yC (y=10, 20, 30, 40, 50, represents number of growth cycles for Cu-HHTP films) towards NH3 and benzene vapor; (d) a response comparison of Cu-TCPP-xC-on-Cu-HHTP-20C (x=0, 5, 10, 15, 20, represents number of transfer cycles for Cu-TCPP films) towards NH3 and benzene vapor; (e) selective change, adapted from the literature [82]; (f) I-V curves of Schottky devices; (g) response-recovery curves of Ag/Cu3(HITP)2/n-Si/Al Schottky device toward 17.38~69.53 mg/m3 NH3; (h) response-recovery curves of Ag/Cu3(HITP)2/n-Si/Al Schottky device toward different gases, adapted from the literature [45]

Figure 10. (a) Schematic and photograph of preparation process of the on-chip micro-biosensor; cyclic voltammogram of (b) US-Cu-BHT film and (c) BS-Cu-BHT film to different concentrations (0~1 mmol/L) of H2O2. Adapted from the literature [87]

Figure 11. (a) Schematic illustration of the preparation process of Ni3(HITP)2/ITO/PET electrode; (b) high magnification SEM; (c) AFM images of Ni3(HITP)2 thin film; (d) CV curves measured at different scan rates; (e) GCD curves measured at different current densities; (f) variation of the areal capacitance versus current density obtained from the GCD curves of Ni3(HITP)2-30 electrode. Adapted from the literature [94]

Figure 12. The electrochemical performance of symmetrical Cu3(HHTP)2 FTSCs: (a) optical transmittance of Cu3(HHTP)2-15 FTCEs and symmetrical FTSCs (Inset: optical image of the bent device); (b) CV curves measured at different scan rates; (c) GCD curves measured at different current densities; (d) cycling performance measured at the current density of 70 µA•cm–2 (Inset: GCD curves at 1st and 3000th cycles); (e) capacitance retention at different bending angles (Inset: CV curves in different bent states); (f) cycling performance measured at the bending angle of 60° (Inset: GCD curves at 1st and 1800th cycles). Adapted from the literature [95]

Figure 13. (a) Perspective view of the two-dimensional layered structure of Ni3(HITP)2; (b) polarization curves of Ni3(HITP)2 under N2 (green) versus O2 atmosphere (red) as well as of the blank glassy carbon electrode under N2 versus O2 atmosphere (blue and purple, respectively). Adapted from the literature [101]

Figure 14. (a) Line profiles corresponding to the inset AFM topography images of a single-layer Co3(HHTP)2 nanosheet; (b) Tafel plots corresponding to different-layer Co3(HHTP)2 LB nanosheet; (c) LSV curves of 4-layer Co3(HHTP)2 nanosheets and RuO2; (d) time dependence of the current density at 1.7 V of 4-layer Co3(HHTP)2 nanosheets (the inset is the enlargement of (d) from 9700 to 9860 s). Adapted from the literature [104]

Figure 15. (a) The crystal structure of [Co3(BHT)2]3– and [Co3(THT)2]3–; (b) polarization curves of MOS1 (red) and MOS2 (blue) in pH=1.3 H2SO4 solution (scan rate: 100 mV/s); adapted from the literature [110]. (c) Schematic diagram to fabricate THTNi thin films; (d) HER polarization plots of the THTNi 2DSP (2D supramolecular polymer) sheet and blank glassy carbon disk electrode in 0.5 mol/L H2SO4 (the inset shows the corresponding Tafel plot). Adapted from the literature [111]

Figure 16. (a) Schematic diagram; (b) transfer curve of Ni3HAB2 thin film FET device; adapted from the literature [114]. (c) Schematic diagram; (d) transfer curve of Ni3(HITP)2 thin film FET device; adapted from the literature [59]; (e) Schematic diagram of liquid-gate Ni3(HITP)2 thin film FET device; (f) Ids-Vgs plots (Vds=–0.1 V) of the Ni-MOF FET exposed to gluconic acid from 10–6 to 10–3 g/mL. adapted from the literature [115]

Figure 17. The 2D EC-MOF-based vertical OSVs with (a) schematic diagram; (b) SEM image of the cross section; (c) magnetic hysteresis loops; (d) the MR loop for the LSMO/Cu3(HHTP)2 (100 nm)/Co OSVs at 10 K; (e) temperature dependence of the MR value. Adapted from the literature [46]

Figure 18. (a) Schematics diagram of human brain memory and synaptic structure; (b) schematics diagram of the MOF-based artificial synaptic device; (c) ∆PSC of MOF-artificial synaptic device array stimulated by radiation light with different wavelengths; (d) the ΔPSC of MOF-artificial synaptic device stimulated by a 420 nm wavelength light spike (Vds=1 V and VG=0 V); (e) the variation of ∆PSC continuously stimulated by 420 nm wavelength light spike. Adapted from the literature [60]

EC-MOF薄膜	合成方法	电导率/(S•cm^–1)	应用	参考文献
Cu₃(HHTP)₂	层层自组装	0.02	气体传感	[44]
Cu₃(HITP)₂	层层自组装	0.2	气体传感	[45]
Cu₃(HHTP)₂	层层自组装	0.29	有机自旋阀	[46]
3D基底Cu₃(HHTP)₂	层层自组装		气体传感	[48]
Cu-CAT	液-液界面法	10^–4		[54]
Ag₃BHT₂ Au₃BHT₂	液-液界面法	363 19.8		[55]
THTA-Co	液-液界面法		电催(HER)	[56]
Ni₃(HITP)₂	气-液界面法	40	FET	[59]
Cu-THPP	气-液界面法		人工突触	[60]
Cu₂[PcM-O₈] (M=Cu或Fe)	气-液界面法	5.6×10^–4		[61]
NiPc-CoTAA	蒸汽辅助转换法	6.67×10^–3	气体传感	[66]
Ni₃(HITP)₂	蒸汽辅助转换法	22.83 (92 nm)		[67]
Cu-BHT	旋涂法		气体传感	[68]
Cu₃(HITP)₂	电化学法	ca. 0.087		[70]
Cu₂(TCPP)	Face-to-Face confinement	ca. 0.007	光电导	[71]
M₃(HHTP)₂ (M=Cu, Co, Ni）	Face-to-Face confinement			[71]
Ni₃(HITP)₂	气-液界面法		超级电容器	[94]
Cu₃(HHTP)₂	层层自组装	0.11	超级电容器	[95]
Ni₃(HITP)₂	溶剂热法	40	电催(ORR)	[101]
Co₃(HHTP)₂	LB结合层层自组装		电催(OER)	[104]
THTNi	气-液界面法		电催(HER)	[111]
Cu-BHT	气-液界面法	1580	FET	[113]
Ni₃HAB₂	液-液界面法		FET	[114]

Table 1. List of partial EC-MOFs thin film with name, synthetic methods, conductivities, and applications

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