PMID- 36677884 OWN - NLM STAT- PubMed-not-MEDLINE DCOM- 20230123 LR - 20230124 IS - 1420-3049 (Electronic) IS - 1420-3049 (Linking) VI - 28 IP - 2 DP - 2023 Jan 13 TI - A Heterostructure Photoelectrode Based on Two-Dimensional Covalent Organic Framework Film Decorated TiO(2) Nanotube Arrays for Enhanced Photoelectrochemical Hydrogen Generation. LID - 10.3390/molecules28020822 [doi] LID - 822 AB - The well-defined heterostructure of the photocathode is desirable for photoelectrochemically producing hydrogen from aqueous solutions. Herein, enhanced heterostructures were fabricated based on typical stable covalent organic framework (TpPa-1) films and TiO(2) nanotube arrays (NTAs) as a proof-of-concept model to tune the photoelectrochemical (PEC) hydrogen generation by tailoring the photoelectrode microstructure and interfacial charge transport. Ultrathin TpPa-1 films were uniformly grown on the surface of TiO(2) NTAs via a solvothermal condensation of building blocks by tuning the monomer concentration. The Pt(1)@TpPa-1/TiO(2)-NTAs photoelectrode with single-atom Pt(1) as a co-catalyst demonstrated improved visible-light response, enhanced photoconductance, lower onset potential, and decreased Tafel slope value for hydrogen evolution. The hydrogen evolution rate of the Pt(1)@TpPa-1/TiO(2)-NTAs photoelectrode was five times that of Pt(1)@TpPa-1 under AM 1.5 simulated sunlight irradiation and the bias voltage of 0 V. A lower overpotential was recorded as 77 mV@10 mA cm(-2) and a higher photocurrent density as 1.63 mA cm(-2). The hydrogen evolution performance of Pt(1)@TpPa-1/TiO(2)-NTAs photoelectrodes may benefit from the well-matched band structures, effective charge separation, lower interfacial resistance, abundant interfacial microstructural sites, and surficial hydrophilicity. This work may raise a promising way to design an efficient PEC system for hydrogen evolution by tuning well-defined heterojunctions and interfacial microstructures. FAU - Zhang, Yue AU - Zhang Y AD - School of Science, China University of Geosciences (Beijing), Beijing 100083, China. FAU - Li, Yujie AU - Li Y AD - School of Science, China University of Geosciences (Beijing), Beijing 100083, China. FAU - Yu, Jing AU - Yu J AD - School of Science, China University of Geosciences (Beijing), Beijing 100083, China. FAU - Sun, Bing AU - Sun B AUID- ORCID: 0000-0001-5917-3094 AD - School of Science, China University of Geosciences (Beijing), Beijing 100083, China. FAU - Shang, Hong AU - Shang H AD - School of Science, China University of Geosciences (Beijing), Beijing 100083, China. LA - eng GR - 2652019113/Fundamental Research Funds for the Central Universities/ GR - 21802128/National Natural Science Foundation of China/ GR - 22001240/National Natural Science Foundation of China/ PT - Journal Article DEP - 20230113 PL - Switzerland TA - Molecules JT - Molecules (Basel, Switzerland) JID - 100964009 SB - IM PMC - PMC9865276 OTO - NOTNLM OT - covalent organic framework OT - heterostructure OT - photocatalytic hydrogen generation OT - surface modification OT - two-dimensional materials COIS- The authors declare no conflict of interest. EDAT- 2023/01/22 06:00 MHDA- 2023/01/22 06:01 PMCR- 2023/01/13 CRDT- 2023/01/21 01:44 PHST- 2022/12/28 00:00 [received] PHST- 2023/01/09 00:00 [revised] PHST- 2023/01/12 00:00 [accepted] PHST- 2023/01/21 01:44 [entrez] PHST- 2023/01/22 06:00 [pubmed] PHST- 2023/01/22 06:01 [medline] PHST- 2023/01/13 00:00 [pmc-release] AID - molecules28020822 [pii] AID - molecules-28-00822 [pii] AID - 10.3390/molecules28020822 [doi] PST - epublish SO - Molecules. 2023 Jan 13;28(2):822. doi: 10.3390/molecules28020822.