摘要
石墨氮化碳(g-C_(3)N_(4))基材料光催化制氢是当前氢能领域的研究热点,但高效g-C_(3)N_(4)材料的设计和合成仍然是一个重大挑战。本工作利用超分子自组装合成策略和水热反应构建了硫掺杂管状g-C_(3)N_(4)/层状ZnIn_(2)S_(4)复合材料,研究了复合材料的光催化性能并揭示机理。结果表明,S掺杂管状g-C_(3)N_(4)具有较大的比表面积、较高的结晶度和较强的还原能力,能够提供足够的反应位点并促进光生电子-空穴转移,与ZnIn_(2)S_(4)形成Ⅱ型异质结后,提升了材料的光吸收能力和光生电子-空穴分离效率,明显增强了光催化制氢性能。10%S掺杂管状g-C_(3)N_(4)/层状ZnIn_(2)S_(4)的产氢速率最高,为1.64 mmol/(g·h),分别是S掺杂管状g-C_(3)N_(4)和层状ZnIn_(2)S_(4)的82倍和2.3倍。
With the continuous growth of global energy demand and the increasing awareness of environmental protection,hydrogen energy,as a clean,efficient,and renewable energy carrier,has received widespread attention.Among various hydrogen production technologies,photocatalytic hydrogen production has become a research hotspot in the field of hydrogen energy due to its use of solar energy to directly decompose water into hydrogen gas,which has the characteristics of being green,efficient,and sustainable.Graphitic carbon nitride(g-C_(3)N_(4)),as a polymer semiconductor photocatalyst,is considered an ideal material for photocatalytic hydrogen production due to its unique physical and chemical properties,such as visible light response,high stability,and low cost.However,how to design and synthesize efficient g-C_(3)N_(4) materials remains a major challenge.On the one hand,the high photogenerated carrier complexation rate of g-C_(3)N_(4) limits its photocatalytic performance;on the other hand,its small specific surface area leads to insufficient photogenerated reaction sites,which further restricts its application in photocatalytic hydrogen production.Therefore,it is of great significance to develop novel structures and composite strategies to optimize the performance of g-C_(3)N_(4).In this paper,a sulfur-doped tubular g-C_(3)N_(4)/lamellar ZnIn_(2)S_(4) composite was successfully constructed using a supramolecular self-assembly synthesis strategy and hydrothermal reaction.By finely tuning the synthesis conditions,the uniform doping of sulfur in tubular g-C_(3)N_(4) was achieved,and a stable type II heterojunction structure was formed with layered ZnIn_(2)S_(4).The experimental results show that sulfur doped tubular g-C_(3)N_(4) has a large specific surface area,providing more active sites for photocatalytic reactions,thereby promoting the generation and transfer of photo generated electron hole pairs,and significantly improving the crystallinity of the material,enhancing its reducing ability,and further improving its photocatalytic performance.When forming a type II heterojunction with ZnIn_(2)S_(4),the light-absorbing ability of the composite was significantly enhanced.This structure not only broadens the light absorption range of the material,but also effectively promotes the separation efficiency of photogenerated electron-hole pairs.In the type II heterojunction,the photogenerated electrons and holes are able to migrate rapidly along the energy band gradient,which reduces the carrier complexation and thus greatly enhances the photocatalytic hydrogen production performance.After systematic testing,the 10%sulfur-doped tubular g-C_(3)N_(4)/layered ZnIn_(2)S_(4) composites exhibit excellent photocatalytic hydrogen production performance with a hydrogen production rate of 1.64 mmol/(g·h).This value is 82 and 2.3 times higher than that of sulfur-doped tubular g-C_(3)N_(4) and layered ZnIn_(2)S_(4) alone,respectively.This significant performance improvement indicates that the bottleneck problem of g-C_(3)N_(4) material in photocatalytic hydrogen production can be effectively improved through morphology control,sulfur doping,and the construction of type II heterojunction strategies,providing new ideas and methods for the development of efficient photocatalytic hydrogen production materials.In the future,further optimization of the structure and composition of the composites is expected to achieve higher photocatalytic hydrogen production efficiency and promote the sustainable development of hydrogen energy technology.
作者
林政楠
方庆艳
谭鹏
陈刚
张成
LIN Zhengnan;FANG Qingyan;TAN Peng;CHEN Gang;ZHANG Cheng(School of Energy and Power Engineering,Huazhong University of Science and Technology,Wuhan 430000,China)
出处
《燃料化学学报(中英文)》
北大核心
2025年第7期1101-1111,共11页
Journal of Fuel Chemistry and Technology
基金
国家自然科学基金(52076090)资助。
作者简介
Corresponding author:张成(1980),男,博士,教授,研究方向为能源相关的先进催化技术,E-mail:chengzhang@hust.edu.cn;林政楠(2001),男,硕士研究生,研究方向为光催化制氢,1259678597@qq.com。
