| 381 | 3 | 105 |
| 下载次数 | 被引频次 | 阅读次数 |
开发利用太阳能解决日益严重的环境危机迫在眉睫,为了提高对太阳光的利用率和光催化剂的性能,采用原位生长并结合表面静电吸附的方法制备三元复合材料,先利用水热合成MoS2/RGO二元异质结复合材料,再根据材料等电点调变溶液pH值制造MoS2与Fe_2O3表面电荷同性、而与RGO表面电荷异性,进而构筑MoS2/RGO/Fe_2O3全固态Z-Scheme光催化剂。通过扫描电镜和透射电子显微镜观察发现,MoS2纳米花球和Fe_2O3纳米颗粒均匀分布在二维片层结构的电子介体RGO表面,MoS2和Fe_2O3分别与RGO形成稳定的异质结构,充分证明此种方式构建复杂三元复合材料的可行性。RGO基全固态Z-Scheme光催化剂在模拟太阳光照射下具有优异的光催化还原降解性能,以无机重金属Cr(VI)溶液作为降解指示剂,60min内全固态Z-Scheme光催化剂中活性最佳的为MR0.43F试样,其光还原降解效率是二元复合材料MoS2/RGO的1.5倍。这种全固态Z-Scheme光催化剂兼具宽光谱吸收、高效光生载流子分离效率和表面化学反应效率,改性后的光催化性能得到显著提升,这一光催化设计路线为水环境处理及清洁能源制备提供了新方向。
Abstract:It is imminent to develop and utilize solar energy to solve the increasingly serious environmental crisis. In order to improve the utilization rate of sunlight and the performance of photocatalysts, this work innovatively proposed to prepare Z-Scheme Mo S2/RGO/Fe_2O3 ternary composites by an in-situ growth method combined with a surface electrostatic adsorption method.MoS2/RGO hetero-structured binary composites were firstly synthesized by a hydrothermal method, and then all-solid-state Z-Scheme MoS2/RGO/Fe_2O3 photocatalyst was constructed via adjusting the solution pH value to create the same charges of MoS_2and Fe_2O3 and the opposite charges of RGO and MoS2. According to the results by scanning electron microscopy and transmission electron microscopy, MoS2 nanosheets and Fe_2O3 nanoparticles are uniformly distributed on the surface of two-dimension RGO, and Mo S2 nanosheets and Fe_2O3 nanoparticles display a stable hetero-structure onto RGO nanosheets. The RGO-based all-solid-state Z-Scheme photocatalyst possesses a superior photocatalytic reduction degradation performance under the simulated solar-driven illumination. Especially, the all-solid-state Z-Scheme photocatalyst MR0.43F has the optimum photoreduction degradation efficiency within 60 min for heavy metal Cr (VI) in a solution as a degradation indicator, which is 1.5 times greater than that of binary Mo S2/RGO composites. The all-solid-state Z-Scheme photocatalyst has wide-spectrum absorption, high separation efficiency of photogenerated carriers and surface chemical reaction efficiency, thus improving the photocatalytic properties.
[1]洪俊明,洪华生,熊小京,等. A/O膜生物反应器组合工艺处理活性染料废水的实验研究[J].厦门大学学报(自然科学版), 2005, 44(3):441-444.HONG Junming, HONG Huasheng, XIONG Xiaojing, et al. J Xiamen Univ(Nat Sci, in Chinese), 2005, 44(3):441-444.
[2] WEI Y Z, WANG J Y, YU R B, et al. Constructing SrTiO3-TiO2heterogeneous hollow multi-shelled structures for enhanced solar water splitting[J]. Angew Chem Int Edit, 2019, 58(5):1436-1440.
[3]程宏飞,赵炳新,张蒙,等.改性高岭石/g-C3N4复合材料光催化性能[J].硅酸盐学报, 2021, 49(7):1367-1376.CHENG Hongfei, ZHAO Bingxin, Zhangmeng, et al. J Chin Ceram Soc, 2021, 49(7):1367-1376.
[4] LEWIS N S, NOCERA D G. Powering the planet:Chemical challenges in solar energy utilization[J]. Natl Acad Sci USA, 2006,103(43):15729-15735.
[5]郑会奇,陈晋,赵杨,等.溶剂热法原位制备TiO2/Ti3C2Tx复合材料及其光催化性能[J].硅酸盐学报, 2020, 48(5):723-729.ZHENG Huiqi, CHEN Jin, ZHAO yang, et al. J Chin Ceram Soc, 2020,48(5):723-729.
[6] UMER M, TAHIR M, AZAM M U, et al. Synergistic effects of single/multi-walls carbon nanotubes in TiO2 and process optimization using response surface methodology for photo-catalytic H2 evolution[J].J Environ Chem Eng, 2019, 7(5):103361.
[7]丁亮,周涵,范同祥.人工无机半导体Z型反应光催化分解水[J].材料导报A, 2013, 27(6):136.DING Liang, ZHOU Han, FAN Tongxiang. Mater Reports(A, in Chinese), 2013, 27(6):136.
[8] XU Q L, ZHANG L Y, CHENG B, et al. S-Scheme Heterojunction Photocatalyst[J]. Chem, 2020, 6(7):1-17.
[9] LU X Y, XIE J, CHEN X B, et al. Engineering MPx(M=Fe, Co or Ni)interface electron transfer channels for boosting photocatalytic H2evolution over g-C3N4/MoS2 layered heterojunctions[J]. Appl Catal B-Environ, 2019, 252(5):250-259.
[10] JANG J S, JANG H G, LEE J S. Heterojunction semiconductors:A strategy to develop efficient photocatalytic materials for visible light water splitting[J]. Catal Today, 2012, 185(1):270-277.
[11] LINSEBIGLER A, LU G, YATES J. Photocatalysis on TiO2 Surfaces:principles, mechanisms, and selected results[J]. Chem Rev, 1995, 95(3):735-738.
[12] LI X, YU J, LOW J, et al. Engineering heterogeneous semiconductors for solar water splitting[J]. J Mater Chem A, 2015, 3(6):2485-2534.
[13] TADA H, MITSUI T, KIYONAGA T, et al. All-solid-state Z-scheme in CdS-Au-TiO2 three-component nanojunction system[J]. Nat Mater,2006(10):782-786.
[14] ZhANG L, WONG K H, CHEN Z, et al. AgBr-Ag-Br2WO6nanojunction system:A novel and efficient photocatalyst with double visible-light active components[J]. Appl Catal A:Gen, 2009, 363(1-2):211-229.
[15] YU Z B, XIE Y P, LIU G, et al. Self-assembled CdS/Au/ZnO heterostructure induced by surface polar charges for efficient photocatalytic hydrogen evolution[J]. J Mater Chem A, 2013, 1(8):2773-2776.
[16] LIU Z, ZHAO Z G, MIYAUCHI M, et al. Efficient visible light active Ca Fe2O4/WO3 based composite photocatalysts:Effect of interfacial modification[J]. Chem C, 2009, 113(39):17132-17137.
[17] HOU J, YANG C, WANG Z, et al. Three-dimensional Z-scheme AgCl/Ag/γ-TaON heterostructural hollow spheres for enhanced visible-light photocatalytic performance[J]. Appl Catal B, 2013,142-143:579-589.
[18] HOU J, CHENG H, TAKEDA O, et al. Threedimensional bimetalgraphene-semiconductor coaxial nanowire arrays to harness charge flow for the photochemical reduction of carbon dioxide[J]. Angew Chem Int Ed, 2015, 54(29):8480-8484.
[19] JIANG J, YU J G, CAO S. Au/PtO nanoparticle-modified g-C3N4 for plasmon-enhanced photocatalytic hydrogen evolution under visible light[J]. Colloid Interface Sci, 2016, 461(1):56-63.
[20] LI A, ZHANG P, CHANG X et al. Gold nanorod@TiO2 yolk-shell nanostructures for visible-light-driven photocatalytic oxidation of benzyl alcohol[J]. Small, 2015, 11(16):1892.
[21] LONG R, LI Y, SONG L, et al. Coupling solar energy into reactions:Materials design for surface plasmon-mediated catalysis[J]. Small,2015, 11(32):3873-3889.
[22] RAJPUT S, CHEN M X, LIU Y, et al. Spatial fluctuations in barrier height at the graphene-silicon carbide Schottky junction[J]. Nat Commun, 2013(4):2752.
[23] CAO S, YU J. Carbon-based H2-production photocatalytic materials[J].Photochem Photobiol C, 2016, 27:72-99.
[24] BAI S, WANG L, CHEN X, et al. Chemically exfoliated metallic MoS2 nanosheets:a promising supporting co-catalyst for enhancing the photocatalytic performance of TiO2 nanocrystals[J]. Nano Res, 2015, 8:175-183.
[25] LUKOWSKI M A, DANIEL A S, MENG F, et al. Highly active hydrogen evolution catalysis from metallic WS2 nanosheets[J]. Energy Environ Sci, 2014, 7(8):2608-2613.
[26] Mahler B, Hoepfner V, Liao K, et al. Colloidal synthesis of 1T-WS2and 2H-WS2 nanosheets:applications for photocatalytic hydrogen evolution[J]. Chem Soc, 2014, 136(40):14121-14127.
[27] SONG S, CHENG B, YU J, et al. Structure effect of graphene on the photocatalytic performance of plasmonic Ag/Ag2CO3-rGO for photocatalytic elimination of pollutants[J]. Appl Cata B, 2016, 181:71-78.
[28] COLEMAN J N. Liquid exfoliation of defect-free graphene[J]. Acc Chem Res, 2013, 46(1):14-22.
[29]姜久兴,闫俊杰,孙宇,等.三维花状Mo S2/Fe2O3纳米异质结构的制备及其光催化性质研究[J].哈尔滨理工大学学报, 2020, 25(3):11-17.JIANG Jiuxing X, Yan Junjie, Sun Yu, et al. J Harbin Univ Sci Technol(in Chinese), 2020, 25(3):11-17.
[30] NITHYA T, SANKEERTHANA B, ARULRA A, et al. Visible light induced efficient hydrogen production through semiconductorconductor-semiconductor(S-C-S)interfaces formed between g-C3N4and rGO/Fe2O3 core-shell composites[J]. Catal Sci Techno, 2018,8(19):5081-5090.
[31] MOTOLA M, BAUDYS M, ZAZPE R, et al. 2D MoS2 nanosheets on1D anodic TiO2 nanotube layers:an efficient co-catalyst for liquid and gas phase photocatalysis[J]. Nanoscale, 2019, 11(48):23126-23131.
[32] CHEN B, MENG Y H, SHA J W. Preparation of Mo S2/TiO2 based nanocomposites for photocatalysis and rechargeable batteries:progress,challenges, and perspective[J]. Nanoscale, 2018, 10:34-68.
[33] WANG S, TANG B W, YANG W L, et al. The flower-like heterostructured Fe2O3/MoS2 coated by amorphous Si-oxyhydroxides:An effective surface modification method for sulfide photocatalysts in photo-fenton reaction[J]. J J Alloys Compd, 2019, 784(5):1099-1105.
[34] GUERRA E, SHANMUGHARAJ A, CHOI W, et al. Thermally reduced graphene oxide-supported nickel catalyst for hydrogen production by propane steam reforming[J]. Appl Catal A, 2013, 468(5):467-474.
[35] ZHANG Y B, TAN Y W, STORMER H L, et al. Experimental observation of the quantum hall effect and Berry's phase in graphene[J].Nature, 2005, 438(7065):201-204.
[36] MEYER J C, GEIM A K, KATSNELSON M I, et al. The structure of suspended graphene sheet[J]. Nature, 2007, 446(7131):60-63.
[37] STANKOVICH S, DIKIN D A, PINER R D, et al. Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide[J]. Carbon, 2007, 45(7):1558-1565.
[38] LIU L, LANG J, ZHANG P, et al. Facile synthesis of Fe2O3 nanodots@nitrogen-doped graphene for supercapacitor electrode with ultralong cycle life in KOH electrolyte[J]. ACS Appl Mater Interfaces,2016, 8(14):9335-9344.
[39] ZHENG X, XU J, YAN K, et al. Space-confined growth of Mo S2nanosheets within graphite:the layered hybrid of MoS2 and graphene as an active catalyst for hydrogen evolution reaction[J]. Chem Mater,2014, 26(7):2344-2353.
[40] ZHAO X, ZHU H, YANG X. Amorphous carbon supported MoS2nanosheets as effective catalysts for electrocatalytic hydrogen evolution[J]. Nanoscale, 2014, 6(18):10680-10685.
[41] ZHANG N, YANG M Q, TANG Z R, et al. Toward improving the graphene semiconductor composite photoactivity via the addition of metal ions as generic interfacial mediator[J]. ACS Nano, 2014, 8(1):623-633.
基本信息:
DOI:10.14062/j.issn.0454-5648.20210792
中图分类号:O643.36;O644.1
引用信息:
[1]焦永欣,王姝,殷佳楠,等.全固态Z-Scheme光催化剂MoS_2/RGO/Fe_2O_3的构筑及性能[J].硅酸盐学报,2022,50(05):1263-1274.DOI:10.14062/j.issn.0454-5648.20210792.
基金信息:
黑龙江省自然科学基金面上项目(E2018042); 广东省联合青年基金项目(2019A1515111019); 理工英才基金项目(LGYC2018JC006)
2022-04-01
2022-04-01
2022-04-01