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MoS2/Zn3In2S6复合光催化剂构建: 高效提升可见光驱动甲酸制氢 被引量:9
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作者 张素娟 段世祥 +5 位作者 陈高礼 孟苏刚 郑秀珍 樊佑 付先亮 陈士夫 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第1期193-204,共12页
虽然传统的化石燃料依然能够满足当今快速工业化发展对能源的巨大需求,但其固有的不可再生性及其燃烧产物对环境的污染,严重阻碍了其在生产和生活中的广泛使用.因此,可持续清洁能源开发的研究已快速成为人类研究的热点.氢是一种具备高... 虽然传统的化石燃料依然能够满足当今快速工业化发展对能源的巨大需求,但其固有的不可再生性及其燃烧产物对环境的污染,严重阻碍了其在生产和生活中的广泛使用.因此,可持续清洁能源开发的研究已快速成为人类研究的热点.氢是一种具备高热值、可持续等优点的清洁能源,也兼备成本及污染低等优势.甲酸(FA)以其无毒、低成本、氢含量高等优点,是一种潜在的热门储氢材料,而可见光占太阳光谱的43%左右.因此,开发高效可见光催化剂驱动FA制氢将是一种应对能源危机的有效途径.许多传统光催化剂已被用于可见光催化FA制氢,但制备成本高、过程复杂、条件苛刻及可见光响应差、稳定性和选择性差、有毒气体释放等缺点严重限制了其光催化性能.光催化研究关键之一是实现光生电荷的高效率分离和转移,从而光催化剂光催化性能的提高.Zn3In2S6(ZIS6)因具有强可见光吸收、稳定性好及环保等特点正迅速成为光催化剂半导体的“明星”,常与助催化剂(如贵金属Pt、Au、Pd等)复合形成异质结以促进光生载流子分离和提高其光催化活性,但制备成本高等因素却严重限制其发展.将成本低、化学稳定性好的MoS2与其它半导体耦合也是提高半导体光催化剂性能的有效手段之一,但高温、热处理时间长及有毒气体释放等却成了制约因素.本文选用价格低廉的反应前驱体,采用简单的一锅法水将MoS2紧密地结合到ZIS6的表面,热制备了一系列含有不同质量百分比MoS2的MoS2/Zn3In2S6(MoS2/ZIS6)复合光催化剂,有效降低了制备成本和有毒气体(H2S)的释放.结果表明,可见光照射下(λ>400 nm),MoS2的引入可大大提高ZIS6光生电荷分离效率及制氢活性,尤其以0.5%MoS2/ZIS6性能最优,光催化制氢速率高达74.25μmol·h^-1(量子效率约2.9%),约ZIS6的4.3倍(17.47μmol·h^-1).XRD结果表明,MoS2/ZIS6样品中含有无定型MoS2紧密固定在晶型ZIS6片状结构表面,未影响ZIS6晶型,SEM表征也证实了此结果.随后的TEM、HRTEM及EDX结果也进一步确认了各组成元素的存在和分布.采用XPS对元素化学环境进行了分析,通过S和Mo元素的成键能变化证实了MoS2和ZIS6间的紧密接触.UV-Vis DRS测试表明,MoS2/ZIS6可以利用可见光在适当带隙的基础上进行光催化制氢.通过BET、PL和电化学技术研究了比表面积、光生电荷分离和传递速率等对光催化性能的影响.最终,结合上述表征结果成功阐述了可见光驱动FA制氢的反应机理. 展开更多
关键词 产氢 Zn3In2S6 甲酸 MOS2 光催化
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g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) S型异质结的自组装制备及其光催化降解诺氟沙星和双酚A
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作者 顾晓蒙 陈太杰 +7 位作者 雷健 杨洋 郑秀珍 张素娟 朱秋实 付先亮 孟苏刚 陈士夫 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第10期2569-2580,共12页
近年来,抗生素的过度使用导致水体严重污染,威胁着生态环境安全和人体健康.太阳光驱动的半导体光催化技术被认为是一种有效去除污染物的手段.由于单一半导体光催化剂的多种缺陷,构建具有可见光响应和强氧化/还原能力的异质结光催化剂是... 近年来,抗生素的过度使用导致水体严重污染,威胁着生态环境安全和人体健康.太阳光驱动的半导体光催化技术被认为是一种有效去除污染物的手段.由于单一半导体光催化剂的多种缺陷,构建具有可见光响应和强氧化/还原能力的异质结光催化剂是去除有机污染物的有效途径.Bi_(8)(CrO_(4))O_(11)(BCO)作为一种新发现的可见光响应半导体,由于较正的价带位,使得其在光催化污染物降解和水氧化方面显示了潜在的应用价值.然而,快速的载流子复合抑制了其活性.石墨相氮化碳(g-C_(3)N_(4),CN)作为不含金属的半导体备受关注,其不仅具有可见光响应、环境友好和电子结构可调等优点,而且二维结构和较负的导带位使得CN更容易与其它半导体形成异质结光催化剂.因此,氧化型的BCO和还原型的CN结合构成异质结,有望形成S型载流子转移,从而提高光生电子-空穴对的分离效率,进而提高光催化降解污染物的活性.本文通过自组装方法制备了一系列新型CN基异质结CN/BCO.CN/BCO异质结光催化降解诺氟沙星(NOR)和双酚A(BPA)的最优比为10%.相对于单体BCO和CN,10%CN/BCO对NOR的降解率分别提高了1.38倍和2.33倍;10%CN/BCO对BPA的降解活性亦得到明显增强,其对BPA的降解率分别是纯BCO和CN的1.35倍和9.11倍.光电流、电化学阻抗谱、稳态荧光和时间分辨瞬态荧光光谱证实了CN/BCO异质结可以显著提升BCO和CN的光生电子-空穴对的分离和迁移效率.原位X射线光电子能谱、电子顺磁共振和自由基捕获实验结果表明,CN/BCO异质结的光催化机制是S型转移.紫外光电子能谱、价带XPS光谱以及载流子浓度等数据进一步揭示了CN/BCO异质结中光生载流子符合S型转移机理的原因.CN作为还原型光催化剂具有较高的费米能级,而BCO作为氧化型光催化剂具有较低的费米能级.此外,CN的载流子浓度大于BCO的载流子浓度.当CN和BCO接触,多子(电子)很容易从CN迁移到BCO,直到它们的费米能级相等.因此,在CN和BCO之间形成了交错的能带结构和由CN指向BCO的内电场,而且在空间电荷区CN的能带向上弯曲,而BCO的能带向下弯曲.当可见光激发CN和BCO产生光生载流子时,在内电场驱动下,BCO导带的电子向CN迁移,CN价带的空穴向BCO迁移;而能带的弯曲和库仑斥力的作用,使得BCO价带的空穴和CN导带的电子各自留在原地.氧化还原能力弱的电子-空穴复合,而保留了空间分离的氧化还原能力强的电子和空穴,形成S型机制,从而显著提高了光催化活性. 展开更多
关键词 Bi_(8)(CrO_(4))O_(11) g-C_(3)N_(4) S型机制 光催化降解 抗生素
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A new phosphidation route for the synthesis of NiPx and their cocatalytic performances for photocatalytic hydrogen evolution over g-C3N4 被引量:2
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作者 Ziqun Wang Longfeng Li +5 位作者 Mingzhu Liu Tifang Miao Xiangju Ye Sugang Meng Shifu Chen xianliang fu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第9期241-249,I0008,共10页
Ni-based phosphides(NiPx)composed of earth-abundant elements are promising cocatalysts to replace noble metals for photocatalytic H2 evolution reaction(HER).A safe,energy-saving,and compositioncontrollable synthesis o... Ni-based phosphides(NiPx)composed of earth-abundant elements are promising cocatalysts to replace noble metals for photocatalytic H2 evolution reaction(HER).A safe,energy-saving,and compositioncontrollable synthesis of NiPx is still highly desired.A facile and mild solvothermal process was developed for the first time for selective synthesis of a series of NiPx,including Ni,Ni12P5,Ni2P/Ni12P5,Ni/Ni2P and Ni2P,through controlling the dosage of NaBH4 and NaH2PO2.The phosphidation process was mainly composed of(1)a sequential reduction of Ni2+to Nj0 and(H2PO2)-to P(around the formed Ni0)triggered by NaBH4,and(2)a final phosphidation between Nj0 and the in situ generated P atoms.The photocatalytic HER performance of g-C3N4 can be substantially improved with the decoration of NiPx(3 wt%)as the separation of photoinduced charge carriers can be promoted and some active sites with low over-potential for HER can be introduced.The cocatalytic efficiency of NiPx is mainly determined by P content.Ni2P with a high ratio of P consequently exhibits the highest HER performance(215.1 umol g-1 h-1),which is almost six times higher than that of the pristine g-C3N4(35.6 umol g-1 h-1).Thus,as for the cocatalyst based on Ni phosphides,Ni2P is the preferable crystal phase and more efforts should be devoted to Ni2P to further optimize its structure,texture,and morphology in future works. 展开更多
关键词 Ni-phosphides Carbon nitrides PHOTOCATALYSIS Hydrogen production Solvothermal synthesis
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A Novel CdS/g-C3N4 Composite Photocatalyst: Preparation, Characterization and Photocatalytic Performance with Different Reaction Solvents under Visible Light Irradiation 被引量:6
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作者 Xiangju Ye Xia Dai +2 位作者 Sugang Meng xianliang fu Shifu Chen 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2017年第2期217-225,共9页
CdS/graphtic carbon nitride (CdS/g-C3N4) hybrid materials were fabricated by thermal polymerization and hy- drothermal methods using Cd(CH3COO)2-2H2O, thioacetamide, and melamine as precursors. The structural and ... CdS/graphtic carbon nitride (CdS/g-C3N4) hybrid materials were fabricated by thermal polymerization and hy- drothermal methods using Cd(CH3COO)2-2H2O, thioacetamide, and melamine as precursors. The structural and op- tical properties of the as-synthesized samples were investigated by X-ray powder diffraction, UV-Vis diffuse reflec- tance spectroscopy, scanning electron microscopy, transmission electron microscopy, etc. A coupled system toward the selective oxidation of benzyl alcohol to benzaldehyde and the reduction of nitrobenzene into aniline was used to estimate the photocatalytic performance of CdS/g-C3N4 composite photocatalysts under visible light illumination. Results indicate that the CdS/g-C3N4 sample exhibits an outstanding photocatalytic performance for selective oxida- tion of benzyl alcohol and reduction of nitrobenzene. Meanwhile, benzotrifluoride is the best reaction medium among the screened solvents. Further research demonstrates that the selective oxidation of benzyl alcohol to ben- zaldehyde is induced by the photoexcited holes and the reduction of nitrobenzene into aniline is triggered by the photoexcited electrons. Additionally, the catalyst can be recycled several times without noticeable deactivation. 展开更多
关键词 CDS g-C3N4 PHOTOCATALYST selective oxidation REDUCTION
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Recent advances in special morphologic photocatalysts for NO_(x)removal 被引量:1
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作者 Yang Yang Xiuzhen Zheng +5 位作者 Wei Ren Jiafang Liu xianliang fu Sugang Meng Shifu Chen Chun Cai 《Frontiers of Environmental Science & Engineering》 SCIE EI CSCD 2022年第11期137-151,共15页
The significant increase of NO_(x)concentration causes severe damages to environment and human health.Light-driven photocatalytic technique affords an ideal solution for the removal of NO_(x)at ambient conditions.To e... The significant increase of NO_(x)concentration causes severe damages to environment and human health.Light-driven photocatalytic technique affords an ideal solution for the removal of NO_(x)at ambient conditions.To enhance the performance of NO_(x)removal,1D,2D and 3D photocatalysts have been constructed as the light absorption and the separation of charge carriers can be manipulated through controlling the morphology of the photocatalyst.Related works mainly focused on the construction and modification of special morphologic photocatalyst,including element doping,heterostructure constructing,crystal facet exposing,defect sites introducing and so on.Moreover,the excellent performance of the photocatalytic NO_(x)removal creates great awareness of the application,which has promising practical applications in NO_(x)removal by paint(removing NO_(x)indoor and outdoor)and pavement(degrading vehicle exhausts).For these considerations,recent advances in special morphologic photocatalysts for NO_(x)removal was summarized and commented in this review.The purpose is to provide insights into understanding the relationship between morphology and photocatalytic performance,meanwhile,to promote the application of photocatalytic technology in NO_(x)degradation. 展开更多
关键词 NO_(x) REMOVAL PHOTOCATALYST Graphene C_(3)N_(4) Bi-based compounds
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