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构建具有微妙的原子级紧密接触的ZnIn_(2)S_(4)/Sv-MoS_(2)光催化剂:增强界面相互作用以改善可见光下的光催化产氢性能

Construction of ZnIn_(2)S_(4)/Sv-MoS_(2)photocatalysts with subtle atomic-level intimate contacts:Enhancing interfacial interactions to improve photocatalytic H2 evolution in visible light
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摘要 催化剂与助催化剂之间的低电荷分离效率严重限制了光催化性能.催化剂与助催化剂之间的强界面相互作用可以提高电荷分离效率.通过引入界面化学键增强组分间的界面相互作用是提高光催化性能的有效手段之一.本文合成了ZnIn_(2)S_(4)(ZIS)/Sv-MoS_(2)光催化剂,ZIS中的S原子与Sv-MoS_(2)中未配位Mo原子之间的键合作用形成了界面Mo–S键,这极大地提高了ZIS的光催化活性.采用不同的NaBH4蚀刻时间制备了MoS_(2-x)h.优化后的Z I S/MoS_(2)-4 h复合材料的产氢速率为7.6 mmol g^(−1)h^(−1),是原ZIS(1.6 mmol g^(−1)h^(−1))的4.75倍,是ZIS/MoS_(2)(3.7 mmol g^(−1)h^(−1))的2.05倍.非凡的光催化活性可归因于光生电子在Mo–S键的作用下更容易从ZIS转移到MoS_(2).光电测量表明,ZIS/MoS_(2)-4h具有有效的电荷转移.本工作揭示了引入界面化学键对ZIS/MoS_(2)光催化活性的影响,为通过界面工程设计优良的助催化剂提供了一种简单有效的方法. The low charge separation efficiency between catalyst and cocatalyst severely limits the performance of photocatalysts.The strong interfacial interactions between catalyst and cocatalyst can improve the charge separation efficiency.Introducing interfacial chemical bonds to enhance the interfacial interaction between components is an effective way to improve photocatalytic performance.Herein,ZnIn_(2)S_(4)(ZIS)/Sv-MoS_(2)photocatalyst was synthesized.The binding effect between S atoms in ZIS and the uncoordinated Mo atoms in Sv-MoS_(2)forms the interfacial Mo–S bond which greatly improves the photocatalytic activity of ZIS.The MoS_(2)-xh was prepared by NaBH4 etching for different times.This extraordinary photocatalytic activity is mainly due to the easy transfer of photogenerated electrons from ZIS to MoS_(2)via the heterojunction interface tightly connected under the action of Mo–S bonds.Photoelectric measurements show that ZIS/MoS_(2)-4h possesses effective charge transfer.This work reveals the effect of the introduction of interfacial chemical bonds on the photocatalytic activity of ZIS/MoS_(2),and provides a simple and effective method for designing excellent cocatalysts through interface engineering.
作者 叶士华 李静君 冯亚男 高水英 曹荣 Shihua Ye;Jingjun Li;Yanan Feng;Shuiying Gao;Rong Cao(State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China;University of the Chinese Academy of Sciences,Beijing 100049,China;Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China,Fuzhou 350108,China)
出处 《Science China Materials》 SCIE EI CAS CSCD 2023年第8期3146-3154,共9页 中国科学(材料科学(英文版)
基金 supported by the National Key Research and Development Program of China(2021YFA1501500) the National Natural Science Foundation of China(22033008,22220102005,and 22171265) Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ103).
关键词 助催化剂 光催化剂 界面相互作用 电荷转移 NABH4 电荷分离 光电测量 原子级 Sv-MoS_(2) ZnIn_(2)S_(4) NaBH4 etching interfacial chemical bond photocatalytic hydrogen evolution
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