Integrating solar-driven water splitting with benzyl alcohol oxidation on ZnIn_(2)S_(4) with Ni-N channel  

利用Ni-N电荷通道促进ZnIn_(2)S_(4)太阳能驱动水分解耦合苯甲醇氧化

作　　者：Hui-Ping Peng Ying-Chen Peng Fei Xue Ye Yang Shang-Heng Liu Xuan Huang Zhong-Liang Huang Lin Sun Hong-Bo Geng Xiao-Qing Huang Yong Xu 彭慧萍;彭应陈;薛飞;杨晔;刘尚恒;黄萱;黄忠亮;孙琳;耿洪波;黄小青;徐勇

机构地区：[1]State Key Laboratory of Physical Chemistry of Solid Surfaces,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China [2]Suzhou Institute of Nano-Tech and Nano-Bionics(SINANO),Chinese Academy of Sciences(CAS),Suzhou 215123,China [3]School of Materials Engineering,Changshu Institute of Technology,Changshu 215500,China

出　　处：《Science China Materials》2025年第3期804-811,共8页中国科学(材料科学)(英文版)

基　　金：supported by the National Key R&D Program of China(2022YFA1504500);National Natural Science Foundation of China(52472310,22025108,U21A20327,and 22121001);Gusu Leading Talent Program(ZXL2024347);Guangdong Provincial Natural Science Fund for Distinguished Young Scholars(2021B1515020081);Pioneer Hundred Talents Program of Chinese Academy of Sciences;Natural Science Foundation of the Jiangsu Higher Education Institutions(22KJA430009);Science and Technology Development Plan of Suzhou(ZXL2022176).

摘　　要：Photocatalytic H_(2) production has been regarded as a charming strategy for harvesting solar energy to chemical energy yet remains a great challenge due to the weak light absorption in visible range,low charge transfer,and fast recombination of photogenerated carriers.Here,we integrate solar-driven water splitting with benzyl alcohol(BA)oxidation,a typical platform chemical from biomass,for producing H_(2) and benzaldehyde(BAD)over ZnIn_(2)S_(4) nanosheets doped with Ni and N(Ni-N/ZIS).Mechanism studies show that Ni-N/ZIS provides a fast charge channel(i.e.,Ni-N)for separating photogenerated electrons and holes,as a result of significantly enhanced photocatalytic performance.Impressively,Ni-N/ZIS displays a H_(2) productivity of 18.7 mmol g^(-1) h^(-1) with an apparent quantum yield(AQE)of 29.1% at 420 nm,which is 37.4,10.6 and 2.8 times higher than that of pristine ZIS,N/ZIS and Ni/ZIS,surpassing all the reported noble metal-free catalysts.Besides,the productivity of BAD reaches 17.5 mmol g^(-1) h^(-1) under the irradiation of visible light(λ≥420 nm).This work integrates two significant processes(i.e.,solar-driven water splitting with benzyl alcohol oxidation)for producing H_(2) and BAD,respectively,which will contribute to alleviating the current energy and environmental crisis.光催化制氢被认为是将太阳能转化为化学能的一种有吸引力的策略,但由于可见光范围内光吸收弱、电荷转移低、光生成载流子的快速重组等问题,仍然面临着巨大的挑战.在这里,我们将太阳能驱动的水分解与苯甲醇(BA)氧化(一种来自生物质的典型平台化学物质)结合起来,在掺杂Ni和N的ZnIn_(2)S_(4)纳米片(Ni-N/ZIS)上生产H_(2)和苯甲醛(BAD).机理研究表明,Ni-N/ZIS为分离光生电子和空穴提供了快速电荷转移通道(Ni-N),从而显著增强了光催化性能.在420 nm处,Ni-N/ZIS的H_(2)产率为18.7 mmol g^(-1) h^(-1),表观量子产率为29.1%,分别是原始ZIS、N/ZIS和Ni/ZIS的37.4倍、10.6倍和2.8倍,超过了所有报道的无贵金属催化剂.在可见光(λ≥420 nm)照射下,苯甲醛的产率达到17.5 mmol g^(-1) h^(-1).本研究将两个重要的工艺(太阳能驱动水分解与苯甲醇氧化)相结合,分别生产H_(2)和BAD,这将有助于缓解当前的能源和环境危机.

关 键 词：Ni-N channel PHOTOCATALYTIC H_(2)evolution benzyl alcohol oxidation efficient charge separation 

分 类 号：O62[理学—有机化学]