Electrochemical water splitting is an important strategy for the mass production of hydrogen. Development of synthesizable catalysts has always been one of the biggest obstacles to replace platinum‐group catalysts. In this work, a high quality crystal polymer covalent triazine framework [CTF; Brunauer–Emmett–Teller (BET) surface area of 1562.6 m2 g−1] is synthesized and MoS2 nanoparticles are grown in situ into/onto the 1 D channel arrays or the external surface for electrocatalysis [hydrogen evolution reaction (HER)] . The state‐of‐the‐art CTFs@MoS2 structure exhibits superior catalytic kinetics with an overpotential of 93 mV and Tafel slope of 43 mV dec−1, which is improved over most other reported analogous catalysts. The inherent π‐conjugated crystal channels in CTFs provides a multifunctional support for electron transmission and mass diffusion during the hydrogen evolution process. Catalytic kinetics analysis shows that the HER performance is closely correlated to the hierarchical pore parameters and aggregated thickness of MoS2 nanoparticles. This work provides an attractive and durable alternative to synthesize high activity and stable catalysts for HER.
Great efforts have been devoted to semiconductive polymers based on the benzo [1,2-b:4,5-b']dithiophene (BDT) unit, and great progress has been achieved in organic solar cells, whereas the analogue core benzo [1,2-b:4,5-b']difuran (BDF) has the similar extended planar structure, and the electronic structure gets less development in the photovoltaic system. Herein, a novel BDF core-based copolymer PBDFTz-SBP is synthesized, which decorates with two 2D extended biphenyl side chains and shows a relatively small polymer segments distortion and strong intermolecular π-π interaction in relation to the BDT-based polymer. Using this polymer, an aggregation-breaking strategy to suppress the trend of self-aggregation of polymers' segment is proposed, which obtains an appropriate phase separation and forms favorable bicontinuous interpenetrating networks for charge transport. It is found that PBDFTz-SBP:ITIC achieves an excellent powerconversion efficiency (PCE) of 12.42% with an open-circuit voltage (V OC ) of 0.89 V, a short-circuit current density (J SC ) of 18.56 mA cm À2 , and a high fill factor (FF) of 75.19% when the spin-coating solution is 120 C, which is higher than that of PBDTTz-SBP:ITIC-based devices even under optimized conditions. This proposed strategy may be a good choice for the BDF unit to construct the donor (D)-acceptor (A) type polymers and surpass the counterpart BDT-based photovoltaic materials and obtain a state-of-the-art PCEs.
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