Oxygen evolution reaction (OER) is a crucial step in many sustainable energy technologies. Exploring cost‐effetive electrocatalysts with high efficiency is one of the most critical but challenging problems to overcome the slow reaction rate and high overpotential in OER. Layered double hydroxide (LDH) has excellent OER performance. However, their poor electrical conductivity and easy agglomeration limit their use. Currently, further phosphorizaton or incorporating with conductive substrates is an effective method to improve the OER performance. In this study, a hybrid product denoted as CoFe−P/Ti3C2Tx were successfully prepared by facile reflux hydrothermal and phosphorization. The optimized CoFe−P/Ti3C2Tx possesses a low overpotential of 270 mV at a current density of 10 mA cm−2 and a small Tafel slope (57.7 mV dec−1). In addition, an overpotential of 337 mV was needed for affording 50 mA cm−2 in the 1 M KOH.

The development of a proton exchange membrane (PEM) that can avoid rapid decay of proton conductivity under low humidity is of great significance for the practical application of PEMFC. In this study, acid–base core–shell microspheres (PCSMs-MA@TAC) with a carboxylic acid core and a triazine shell were synthesized by distillation-precipitation polymerization using cross-linked carboxylic acid microspheres (PMAA) as seeds. These PCSMs were then incorporated into a sulfonated poly(ether ether ketone) matrix to make hybrid membranes. Incorporation of PCSMs microspheres can not only strengthen the vehicle mechanism by increasing the water uptake of the membrane, but also the acid–base pairs formed at the SPEEK/PCSMs interface provide a new low-energy barrier pathway for proton hopping, thereby enhancing the proton conduction of the Grotthuss mechanism. The results show that when the content is 10 wt%, the proton conductivity of the SPEEK/PCSMs-MA@TAC composite membrane can reach 0.161 S cm−1 at 80°C and 100% RH, which is 19.3% higher than the SPEEK control membrane (0.135 S cm−1). In particular, even at 60% RH, the proton conductivity of the SPEEK/PCSMs-MA@TAC-10 composite membrane is still 67 mS cm−1, which is 3.16 times higher than that of the SPEEK membrane. Therefore, the SPEEK/PCSMs-MA@TAC composite membrane can maintain superior performance even under high temperature and low humidity conditions.

Sulfonated poly(ether ether ketone) (SPEEK) has been widely investigated as a substitution of commercial Nafion as proton exchange membranes (PEMs). However, the disadvantages such as shrinkage of proton transfer channels at high temperature and low humidity conditions cannot be neglected. In this manuscript, the carboxyl and imidazole double‐shelled carbon nanotubes(CNTs−C@N) was incorporated into the SPEEK matrix to fabricate composite PEM (denoted as SPEEK/CNTs−C@N−Y, Y is the percentage composition of CNTs−C@N), serving as one‐dimensional fillers. SPEEK/CNTs−C@N‐1.0 composite membrane performed a higher horizontal proton conductivity (0.302 S/cm) under 80 °C and 100 % relative humidity (RH) compared with original SPEEK membrane 0.181 S/cm. The high proton conductivity could be mainly attributed to the dual proton conducting channel formed by two types of acid‐base pairs, which immensely promote the Grotthuss mechanism. Therefore, SPEEK/CNTs−C@N composite membranes are expected to develop PEMs with high proton conductivity at high temperature and low humidity.