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Efficient CO 2 electrodes require optimized catalytic activity and a delicate electrode structure. However, it is often insufficient to consider only a single factor when constructing a high-performance electrode. In this study, we elaborately prepare the freestanding Fe-doped CoP catalysts on N-doped carbon cloth (Fe-CoP@N-CC) substrates, which synergistically realizes electronic structure tuning of the catalysts and electrode structure modification. The experimental and theoretical calculations reveal that the electrode structure, consisting of fully covered nanowires on an N-CC skeleton, promotes mass transfer and accommodates products. The introduction of N atoms in Fe-CoP@N-CC leads to increased defects and strong Co–N–C bonds at the interface, enhancing interfacial electron transfer. Furthermore, Fe doping optimizes the electronic structure of Fe-CoP@N-CC. This synergistic enhancement facilitates the kinetics of both CO 2 reduction reaction (CO 2 RR) and CO 2 evolution reaction (CO 2 ER), resulting in the formation of large-size spherical morphologies following the solution pathway. The improved electrocatalytic performance of Fe-CoP@N-CC electrodes was demonstrated by their high discharge capacity of 4127 mAh g−1 and cycling stability of 446 h in Li–CO 2 batteries. These findings emphasize the significance of compatibility between electrode structure and catalytic activity in the design of CO 2 electrode. • Fe-doped CoP on N-doped carbon cloth (Fe-CoP@N-CC) substrates were fabricated. • Enlarged reaction active area and promoted mass transfer. • Strong Co–N–C bonds at the interface can facilitate interfacial electron transfer. • Enhanced CO 2 RR and CO 2 ER kinetics are realized. • Optimizing morphology and discharge product pathways. [ABSTRACT FROM AUTHOR]

• The Ni 2 P/CTF photocatalyst prepared by solid state chemical reduction method. • The H 2 evolution rate for 2.8%Ni 2 P/CTF is almost the same as that of 3.0%Pt/CTF. • The Ni 2 P cocatalysts act as active centers for H 2 evolution of CTF photocatalyst. [Display omitted] The covalent triazine frameworks (CTFs) have recently become a new generation of organic semiconductor for photocatalytic hydrogen production from water splitting because of their great application potentials. However, the CTFs need to be combined with noble-metal-cocatalysts to achieve photocatalytic water splitting. Herein, we reported the noble-metal-free Ni 2 P/CTF composites as an efficient catalyst for photocatalytic hydrogen evolution. With increasing the Ni 2 P alloy loading on the surface of CTF, the photocatalytic activity increases obviously and then decreases gradually, and the highest photocatalytic H 2 evolution rate is achieved for 2.8%Ni 2 P/CTF, which is almost the same as that of 3.0%Pt/CTF photocatalyst. It has been revealed that the Ni 2 P alloy act as a cocatalyst for effectively suppressing the recombination of photogenerated electrons and holes, promoting the separation and migration of the charge carriers, thereby improving the efficiency of photocatalytic H 2 evolution. This work provides a promising strategy for preparation of cheap and stable photocatalytic system based on CTF for efficient photocatalytic hydrogen evolution under visible-light irradiation. [ABSTRACT FROM AUTHOR]