Thinned g-C3N4 nanosheets with microdopants of cucurbit[7]uril to improve photoelectrochemical water-splitting

IF 4.1 3区 化学 Q2 CHEMISTRY, PHYSICAL
Hong-Si Guo , Wenfeng Zhao , Wan-Ling Chen , Qingmei Ge , Mao Liu , Hang Cong , Jiang-Lin Zhao
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Abstract

Utilizing solar energy to generate hydrogen through photoelectrochemical (PEC) water splitting is considered as the most efficient method and sustainable pathway. Graphitic carbon nitride (g-C3N4), as a candidate for photoelectrochemical catalysts, exhibits the drawbacks including small specific surface area and high complexity of photogenerated electron-hole pairs. With supramolecular encapsulation of melamine guest within cucurbit[7]uril, a new process for thinned and nitrogen-doped g-C3N4-0.04 % nanosheets are developed, and the photoelectrocatalytic activity is obviously improved on the surface. A photocathode with the prepared g-C3N4-0.04 % nanosheets produce more than twice efficiency of pristine g-C3N4 for water splitting, and the incident photon-to-current conversion efficiency (IPCE) is increased by a factor of about 10 under simulated conditions of sunlight at AM 1.5 G (100 mW/cm2). The improved performance should be the results of the thinned layers by introduction of the macrocyclic compound in g-C3N4 nanosheets, which reduce the charge transfer resistance, and inhibit the complexation of the photogenerated electron pairs, to prolong the lifetime of the electron, and facilitate the ability of the electron transport with an increase in current. On the other hand, the specific surface area is improved in the g-C3N4-0.04 % nanosheets to expose more reactive sites, and the microdopant of cucurbit[7]uril provides more active nitrogen sites, to enhance the photocatalysis.

Abstract Image

含有葫芦[7]脲微掺杂剂的稀化 g-C3N4 纳米片改善光电化学分水性能
利用太阳能通过光电化学(PEC)分水产生氢气被认为是最有效的方法和可持续的途径。氮化石墨碳(g-C3N4)作为光电化学催化剂的候选材料,具有比表面积小、光生成的电子-空穴对复杂性高等缺点。通过将三聚氰胺客体超分子封装在葫芦[7]脲中,开发出了一种减薄和氮掺杂 g-C3N4-0.04 % 纳米片的新工艺,并明显提高了其表面的光电催化活性。在 AM 1.5 G(100 mW/cm2)的模拟太阳光条件下,使用制备的 g-C3N4-0.04 % 纳米片的光电阴极的水分离效率是原始 g-C3N4 的两倍多,入射光子到电流的转换效率(IPCE)提高了约 10 倍。性能的提高应该是 g-C3N4 纳米片中引入大环化合物使层变薄的结果,从而降低了电荷转移电阻,抑制了光生电子对的络合,延长了电子的寿命,并随着电流的增加促进了电子传输能力。另一方面,g-C3N4-0.04 % 纳米片的比表面积得到改善,暴露出更多的反应位点,葫芦[7]脲的微掺杂剂提供了更多的活性氮位点,从而增强了光催化能力。
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来源期刊
CiteScore
7.90
自引率
7.00%
发文量
580
审稿时长
48 days
期刊介绍: JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds. All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor). The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.
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