Li YZheng TLiu YDall'Agnese YDall'Agnese CLiu C.-LSasaki S.-ITamiaki HWang X.-F.CHENG-LIANG LIU2022-03-222022-03-22202203603199https://www.scopus.com/inward/record.uri?eid=2-s2.0-85120401532&doi=10.1016%2fj.ijhydene.2021.11.026&partnerID=40&md5=616dfe85ccac19277bd81220a56a38d3https://scholars.lib.ntu.edu.tw/handle/123456789/598345Development of efficient photocatalytic hydrogen evolution reaction (HER) with illumination of visible light is challenging. In this work, five chlorophyll derivatives (M-Chls; M = H2/Cu/Ni/Co/Zn) with different central ions in its cyclic tetrapyrrole ring including free base, copper, nickel, cobalt, and zinc were synthesized and employed as the effective visible-light harvester for efficient HER. In addition, two-dimensional (2D) noble metal-free co-catalyst Ti3C2Tx MXene was used as an excellent electron capturer due to its outstanding conductivity property. These M-Chls are modified on the surface of Ti3C2Tx MXene with 2D accordion-like morphology by means of a simple deposition process to form noble metal-free Chl/Ti3C2Tx-based photocatalysts for HER. It is found that the best HER performance as high as 49 μmol/h/gcat was achieved with the Co-Chl@Ti3C2Tx hybrid, which was much higher than those of other M-Chl@Ti3C2Tx composites. This research provides a specific way to synthesize low-cost and environmentally friendly natural Chls for developing highly efficient photocatalytic HER through molecular engineering. ? 2021 Hydrogen Energy Publications LLCAggregates materialsCentral metals ionChlorophyll derivativesHydrogen evolution reactionTi3C2Tx MXeneChlorophyllCost engineeringHeavy metalsHydrogenLightPhotocatalytic activityPrecious metalsAggregate materialsCentral metal ionCentral metalsChlorophyll derivativeHydrogen evolution reactionsMetal freeMetals ionsPhotocatalytic hydrogen evolutionTi3C2Tx mxeneVisible lightMorphologyjournal article10.1016/j.ijhydene.2021.11.0262-s2.0-85120401532