Molecular-doped Precursor Derived Porous g-C₃N₄ for Photocatalytic H₂ Production

Abstract

Molecular design of novel precursors represents a strategic approach to mitigating severe charge recombination in g-C₃N₄. Distinct from conventional high-temperature thermal polymerization, this work develops novel precursors through low-temperature hydrothermal assembly of melamine-cyanuric acid supramolecule with hexamethylenetetramine doping. After the calcination of modified precursors, the obtained g-C₃N₄ has a porous structure and an ultra-high specific surface area. Advanced characterizations confirm the reduced layer stacking, the disrupted π-π conjugated structure, and critically, the accelerated charge transport efficiency. Remarkably, the modified g-C₃N₄ achieves a 22 times enhancement in visible-light-driven hydrogen evolution (λ>400 nm) compared to pristine g-C₃N₄, which is among the highest improvements reported for supramolecular modified g-C₃N₄ systems. This molecular engineering strategy for precursors establishes a new approach to designing high-performance photocatalysts.

Keywords

Graphite carbon nitride / Photocatalysis / Hydrogen / Supramolecule

References

[1] GongB L, MaX Q, WangT G, HouJ L, JiS X, XuQ J, CaoH JAdv. Colloid Interface Sci., 2024, 336103373.

[2] AllakhverdievS IInt. J. Hydrogen Energy, 2024, 90199.

[3] HuoR, LiM, ZhengW B, MingP W, LiB, ZhangC M, LiZ LEnerg. Convers. Manage., 2024, 317118819.

[4] SainiP, KumarK, SainiS, SethiM, MeenaP, GurjarA, WeigandW, ParewaVCoord. Chem. Rev., 2024, 502215607.

[5] BelousovA S, ShafiqIJ. Environ. Chem. Eng., 2023, 11110970.

[6] IervolinoG, ZammitI, VaianoV, RizzoLTop. Curr. Chem., 2020, 378225

[7] FujishimaA, HondaKNature, 1972, 23837.

[8] FuC H, LiD, ZhangJ W, GuoW, YangH, ZhaoB, ChenZ M, FuX, LiangZ Q, JiangLChem. Res. Chinese Universities, 2023, 39891.

[9] LiZ, LiR G, JingH J, XiaoJ P, XieH C, HongF, TaN, ZhangX W, ZhuJ, LiCNat. Catal., 2023, 680.

[10] LinJ K, TianW J, GuanZ Y, ZhangH Y, DuanX G, WangH, SunH Q, FangY F, HuangY P, WangS BAdv. Funct. Mater., 2022, 322201743.

[11] JiH Q, LiuY X, DuG Y, HuangT Y, ZhuY, SunY Y, PangHChem. Res. Chinese Universities, 2024, 40943.

[12] NiuQ, MiL H, ChenW, LiQ J, ZhongS H, YuY, LiL YChin. J. Catal., 2023, 5045.

[13] QianY T, ZhangF F, KangD J, PangHEnergy Environ. Mater., 2023, 6e12414.

[14] LiT, TsubakiN, JinZ LJ. Mater. Sci. Technol., 2024, 16982.

[15] MengC C, HuangM, LiY CChem. Res. Chinese Universities, 2023, 39697.

[16] YuK, ZhangC, ChangY, FengY, YangZ, YangT, LouL-L, LiuSAppl. Catal. B-Environ., 2017, 200514.

[17] OngW-J, TanL-L, NgY H, YongS-T, ChaiS-PChem. Rev., 2016, 1167159.

[18] HayatA, TahaT, AlenadA M, UllahI, ShahS J A, UddinI, UllahI, HayatA, KhanW USurf. Interfaces, 2021, 25101166.

[19] JoW-K, TondaSJ. Hazard. Mater., 2019, 368778.

[20] FeiH, ShaoJ X, LiH, LiN J, ChenD Y, XuQ F, HeJ H, LuJ MAppl. Catal. B-Environ., 2021, 299120623.

[21] MaoL H, ZhaiB J, WenL Y, XiaoW B, ShiJ W, KangX, LiuY B, ChengC, JinH, GuoL JAppl. Catal. B-Environ., 2025, 362124712.

[22] ChengC, ShiJ W, MaoL H, DongC-L, HuangY-C, ZongS C, LiuJ M, ShenS H, GuoL JJ. Colloid Interf. Sci., 2023, 637271.

[23] MaoL H, ZhaiB J, ShiJ W, KangX, LuB R, LiuY B, ChengC, JinH, LichtfouseE, GuoL JACS Nano, 2024, 1813939.

[24] KangX, JiangY Z, ShiJ W, MaoL H, LiuY B, ZhaiB J, JinH, GuoL JJ. Colloid Interf. Sci., 2025, 685716.

[25] Abou SaoudW, BelkessaN, AzzazA A, RochasV, MezinoV, PressetM-A, LechevinS, GenouelA, RouxelS, MonsimertDChem. Eng. J., 2023, 468143710.

[26] AcarE G, KoçB K, IsrarM, AslanE, AltanO, Patirİ H H, MetinÖJ. Environ. Chem. Eng., 2025, 13115343.

[27] LvX T, JinX L, MengJ W, YangK T, LinS L, HaoW X, ZhaoM Y, WangH Q, ZhangX H, LvC D, XieH QJ. Colloid Interf. Sci., 2025, 6861009.

[28] KeY L, YouQ L, AiJ, YangX F, ShangQ G, LiuY Y, WangD S, LiaoG YJ. Mater. Sci. Technol., 2023, 15237.

[29] YinF X, QinP Q, XuJ S, CaoS WActa Phys. -Chimi. Sin., 2023, 392212062.

[30] ChenG Q, ZhengZ X, ZhongW, WangG H, WuX HActa Phys.-Chimi. Sin., 2024, 402406021.

[31] LiuX L, ZhangQ Q, CuiZ H, MaF H, GuoY H, WangZ Y, LiuY Y, ZhengZ K, ChengH F, DaiY, HuangB B, WangPInt. J. Hydrogen Energy, 2022, 4718738.

[32] ChenS, WenX Y, ChenY L, XiaZ Y, ChenQ R, HuangL L, HuangH N, PanH W, FuY L, HeJ R, LiW SChem. Engin. J., 2024, 479147813.

[33] JiangZ C, LongQ, ChengB, HeR A, WangL XJ. Mater. Sci. Technol., 2023, 1621.

[34] ZhongR Y, LiangY J, HuangF, LiangS N, LiuS WChin. J. Catal., 2023, 53109.

[35] ChenY L, LiuX Q, HouL, GuoX R, FuR W, SunJ MChem. Eng. J., 2020, 383123132.

[36] LiY-Y, ZhouB-X, ZhangH-W, MaS-F, HuangW-Q, PengW, HuW, HuangG-FNanoscale, 2019, 116876.

[37] MaoL H, ChenK L, JiangY Z, KangX, ZhangY Z, ChengC, ChenY, ShiJ WSustainable Energy Fuels, 2025, 91498.

[38] LiuQ, WangX L, YangQ, ZhangZ G, FangX MAppl. Surf. Sci., 2018, 45046.

[39] DuJ G, XuZ, LiH, YangH J, XuS J, WangJ, JiaY N, MaS L, ZhanS HAppl. Surf. Sci., 2021, 541148487.

[40] ZouJ, LiaoG D, JiangJ Z, XiongZ G, BaiS S, WangH T, WuP X, ZhangP, LiXChin. J. Struct., 2022, 412201025

[41] ZhongL, YingM F, MouZ G, LuoR, SunJ H, LiuD, LeiW WJ. Colloid Interf. Sci., 2022, 612479.

[42] LiY H, HeZ J, LiuL, JiangY, OngW J, DuanY Y, HoW K, DongFNano Energy, 2023, 105108032.

[43] ZhaiB J, LiY, JiangY Z, MaoL H, ShiJ W, ZhaoQ Q, BinZ D, WangF Y, DuY P, JinHJ. Colloid Interf. Sci., 2025, 6851099.

[44] YangY, LiuJ J, GuM L, ChengB, WangL X, YuJ GAppl. Catal. B-Environ., 2023, 333122780.

[45] XueY J, ZhaoG Y, ZhangW Q, ZhaoJ S, MengF P, ZhaoFACS Appl. Polym. Mater., 2024, 611444.

[46] MaoL H, LuB R, ShiJ W, ZhangY Z, KangX, ChenY B, JinH, GuoL JCatalysis Today, 2023, 40994.

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Jilin University, The Editorial Department of Chemical Research in Chinese Universities and Springer-Verlag GmbH

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