A series of composite cross-linked membrane based on fluorine-containing polybenzimidazole (6FPBI) and a cross-linkable polymeric ionic liquid (cPIL) have been prepared for high temperature proton exchange membrane (HT-PEM) applications. Particularly, the obtained composite cross-linked membranes showed excellent phosphoric acid doping ability and proton conductivity. On the basis of the trade-off between mechanical strength and proton conductivity of composite membranes, the optimal content of cPIL is 20 wt % (6FPBI-cPIL 20 membrane). For instance, the 6FPBI-cPIL 20 membrane with a PA doping level of 27.8 exhibited a proton conductivity of 0.106 S cm −1 at 170 °C, which is much higher than that of pristine 6FPBI membrane. The most outstanding contribution of this work is that the 6FPBI-cPIL membranes showed improved phosphoric acid retention and long-term conductivity stability under harsh conditions (80 °C/40% RH) for 96 h. In particular, the proton conductivity and PA doping level of the 6FPBI-cPIL 20 membrane remained at a high level of 0.064 S cm −1 and 8.5 after 96 h of the test, respectively.

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The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202100762. conversion are potential methods to lower CO 2 concentration in the atmosphere. [2][3][4] In contrast to CO 2 capture, CO 2 conversion is more promising, as it can convert CO 2 into low-carbon fuels or other valuable chemicals such as CO, CH 4 , HCOOH, and C 2 H 5 OH. [5][6][7][8] Importantly, for industrial applications, CO 2 reduction reaction (CO 2 RR) is considered to be a practical and potentially valuable method for the generation of clean, renewable energy that can be undertaken even at room temperature and ambient pressure. [9][10][11][12][13] Given the high thermodynamic stability, the low electron affinity of CO 2 molecules, and the competitive reaction of hydrogen evolution in the formation of the desired products, a highly selective and efficient catalyst for CO 2 RR is urgently needed. [14][15][16][17][18][19][20][21] In recent years, metal-organic frameworks (MOFs) composed of various transition metals ions and organic linkers have emerged in the field of electrocatalysis. [22,23] Compared with noble metals, transition metal chalcogenides, and other catalytic materials, MOFs feature very large specific surface