C/TiO2-SO42-的制备及其光解水性能

doi:10.11949/j.issn.0438-1157.20170308

摘要/Abstract

摘要：

通过溶胶-凝胶制备过程中水含量控制，分别获得了硫酸根修饰的TiO₂（25）和无修饰的TiO₂（150）两种二氧化钛载体。在两种载体上，通过浸渍法引入不同浓度的碳点胶体，获得了系列不同C含量的C_x/TiO₂（25）和C_x/TiO₂（150）催化剂。利用TEM、XRD、FT-IR、UV-Vis、BET、XPS等表征分析了催化剂的表面形貌、晶格间距、晶型结构、光吸收、孔结构及元素组成。结果显示：相对于无硫酸根修饰的TiO₂（150）催化剂，硫酸根修饰的TiO₂（25）催化剂的光吸收发生显著红移，展示了更宽的可见光响应；对于TiO₂（25）样品，C的引入可提高其O_ads/O_latt比值。催化性能研究显示，C的引入可以提高其光催化活性。

关键词: 硫酸根, 复合材料, 纳米材料, 催化剂, 碳点, 光催化, 制氢

Abstract:

The SO₄^2- modified TiO₂(25) and the unmodified TiO₂(150) have been prepared by sol-gel method via controlling the amount of introduced deionized water. Two series of C modified C_x/TiO₂(25) and C_x/TiO₂(150) samples were obtained by impregnating the TiO₂(25) and TiO₂(150) in carbon dots solution with various concentrations. The lattice spacing, crystalline, light absorption, pore size, specific surface area and element composition of the prepared catalysts were characterized by TEM, XRD, FT-IR, UV-Vis, BET and XPS. The results indicated that compared with the unmodified TiO₂(150), the SO₄^2- modified TiO₂(25) exhibited a distinct red shift phenomenon and broader visible light response for the light absorption. Moreover, the O_ads/O_latt ratios can be improved distinctly for the TiO₂(25) when the carbon dots were introduced. The catalytic performance showed that the addition of C can enhance the corresponding photocatalytic activity.

Key words: SO₄^2-, composites, nanomaterials, catalyst, carbon dots, photocatalytic, hydrogen production

中图分类号:

O611

滕雪刚, 杨仁春, 任超, 刘璐璐, 汪明星. C/TiO₂-SO₄^2-的制备及其光解水性能[J]. 化工学报, 2017, 68(11): 4414-4422.

TENG Xuegang, YANG Renchun, REN Chao, LIU Lulu, WANG Mingxing. Preparation of C/TiO₂-SO₄^2- and their water splitting performance[J]. CIESC Journal, 2017, 68(11): 4414-4422.

参考文献 41

[1]	申玉芳, 龙飞, 邹正光. 半导体光催化技术研究进展[J]. 材料导报, 2006, 20(6):28-31. SHEN Y F, LONG F, ZOU Z G. Developments of photocatalytic semiconductors[J]. Mater. Rev., 2006, 20(6):28-31.
[2]	FUJISHIMA A, HONDA K. Electrochemical photolysis of water at a semiconductor electrode[J]. Nature, 1972, 37:38-245.
[3]	DEMIRCI S, DIKICI T, YURDDASKAL M, et al. Synthesis and characterization of Ag doped TiO2 heterojunction films and their photocatalytic performances[J]. Appl. Surf. Sci., 2016, 390:591-601.
[4]	BANERJEE A N, HAMNABARD N, SANG W J. A comparative study of the effect of Pd-doping on the structural, optical, and photocatalytic properties of sol-gel derived anatase TiO2 nanoparticles[J]. Ceram. Int., 2016, 42:12010-12026.
[5]	LI D, CHEN F, JIANG D L, et al. Enhanced photocatalytic activity of N-doped TiO2 nanocrystals with exposed {001} facets[J]. Appl. Surf. Sci., 2016, 390:689-695.
[6]	LIN Y H, CHANG C W, CHU H, et al. The visible light-driven photodegradation of dimethyl sulfide on S-doped TiO2:characterization, kinetics, and reaction pathways[J]. Appl. Catal. B:Environ., 2016, 199:1-10.
[7]	WANG Y Z, WU Y S, YANG H, et al. Doping TiO2 with boron or/and cerium elements:effects on photocatalytic antimicrobial activity[J]. Vacuum, 2016, 131:58-64.
[8]	CHENG Z W, GU Z Q, CHEN J M. Synthesis, characterization, and photocatalytic activity of porous La-N-co-doped TiO2 nanotubes for gaseous chlorobenzene oxidation[J]. J. Environ. Sci.-China, 2016, 46:203-213.
[9]	DU C, ZHOU J S, LI F Z, et al. Extremely fast dark adsorption rate of carbon and nitrogen co-doped TiO2 prepared by a relatively fast, facile and low-cost microwave method[J]. Appl. Phys. A, 2016, 122:714.
[10]	MOYA A, CHEREVAN A, MARCHESAN S, et al. Oxygen vacancies and interfaces enhancing photocatalytic hydrogen production in mesoporous CNT/TiO2, hybrids[J]. Appl. Catal. B:Environ., 2015, 179:574-582.
[11]	TIAN J, LENG Y H, ZHAO Z H, et al. Carbon quantum dots/hydrogenated TiO2 nanobelt heterostructures and their broad spectrum photocatalytic properties under UV, visible, and near-infrared irradiation[J]. Nano Energy, 2015, 11:419-427.
[12]	YU X J, LIU J J, YU Y C, et al. Preparation and visible light photocatalytic activity of carbon quantum dots/TiO2 nanosheet composites[J]. Carbon, 2014, 68:718-724.
[13]	FUJITA SI, KAWAMORI H, HONDA D, et al. Photocatalytic hydrogen production from aqueous glycerol solution using NiO/TiO2 catalysts:effects of preparation and reaction conditions[J]. Appl. Catal. B:Environ., 2016, 181:818-824.
[14]	NIU W, WANG G, LIU X D, et al. Preparation of WO3-TiO2 photo-anode and its performance of photocatalytic hydrogen production by water splitting[J]. Int. J. Electrochem. Sc., 2015, 10:8513-8521.
[15]	TANIGAWA S, IRIE H. Visible-light-sensitive two-step overall water-splitting based on band structure control of titanium dioxide[J]. Appl. Catal. B:Environ., 2016, 180:1-5.
[16]	LIM S Y, SHEN W, GAO Z Q. Carbon quantum dots and their applications[J]. Chem. Soc. Rev., 2015, 44:362.
[17]	PIZEM H, SUKENIKC N, SAMPATHKUMARAN U, et al. Effects of substrate surface functionality on solution-deposited titania films[J]. Chem. Mater., 2002, 14:2476-2485.
[18]	沈俊, 罗妮, 张明俊, 等. 介孔TiO2-SO42-的合成及表征[J]. 催化学报, 2007, 28(3):264-268. SHEN J, LUO N, ZHANG M J, et al. Synthesis and characterization of mesoporous TiO2-SO42-[J]. Chinese J. Catal., 2007, 28(3):264-268.
[19]	唐守强, 何菁萍. 介孔SO42-/TiO2粉体的制备及光催化性能的研究[J]. 硅酸盐通报, 2011, 30(6):1404-1409. TANG S Q, HE J P. Study on preparation and photocatalytic capability of mesoporous SO42-/TiO2[J]. Bull. Chinese Ceram. Soc., 2011, 30(6):1404-1409.
[20]	苏文悦, 付贤智. 光催化剂SO42-/TiO2和TiO2的光谱行为比较[J]. 光谱学与光谱分析, 2000, 20(5):655-657. SU W Y, FU X Z. Comparison of spectral behavior of SO42-/TiO2 and TiO2 photocatalyst[J]. Spectrosc. Spect. Anal., 2000, 20(5):655-657.
[21]	彭少洪, 张渊明, 钟理. TiO2基固体超强酸的制备及光催化性能研究[J]. 无机化学学报, 2006, 34(12):2258-2262. PENG S H, ZHANG Y M, ZHONG L. Preparation of TiO2-based solid superacid and its photocatalytic performance[J]. J. Inorg. Mater., 2006, 34(12):2258-2262.
[22]	YUAN H, HE J, LI R, et al. Characterization of SO42-/TiO2 and its catalytic activity in the epoxidation reaction[J]. Res. Chem. Intermed., 2017, 43:4353-4368.
[23]	MENG C, CAO G P, LI X K, et al. Structure of the SO42-/TiO2 solid acid catalyst and its catalytic activity in cellulose acetylation[J]. Reac. Kinet. Mech. Cat., 2017, 121:719-734.
[24]	VELMURUGAN R, KRISHNAKUMAR B, SWAMINATHAN M. Synthesis of Pd co-doped nano-TiO2-SO42-, and its synergetic effect on the solar photodegradation of Reactive Red 120 dye[J]. Mat. Sci. Semicon. Proc., 2014, 25(25):163-172.
[25]	FERNANDO K A, SAHU S, LIU Y, et al. Carbon quantum dots and applications in photocatalytic energy conversion.[J]. ACS Appl. Mater. Inter., 2015, 7(16):8363.
[26]	ZALFANI M, SCHUEREN B V D, MAHDOUANI M, et al. ZnO quantum dots decorated 3DOM TiO2, nanocomposites:symbiose of quantum size effects and photonic structure for highly enhanced photocatalytic degradation of organic pollutants[J]. Appl. Catal. B:Environ., 2016, 199:187-198.
[27]	WANG X W, SUN G Z, LI N, et al. Quantum dots derived from two-dimensional materials and their applications for catalysis and energy[J]. Chem. Soc. Rev., 2016, 47(22):2239.
[28]	CHEN T, QUAN W, YU L, et al. One-step synthesis and visible-light-driven H2 production from water splitting of Ag quantum dots/g-C3N4 photocatalysts[J]. J. Alloy. Compd., 2016, 686:628-634.
[29]	GUTIÉRREZ O Y, PÉREZ F, FUENTES G A, et al. Deep HDS over NiMo/Zr-SBA-15 catalysts with varying MoO3 loading[J]. Cataly. Today, 2008, 130(2/3/4):292-301.
[30]	YANG R C, ZHANG Z H, REN Y M, et al. Green synthesis of bi-component copper oxide composites and enhanced photocatalytic performance[J]. Mater. Sci. Tech-Lond., 2015, 31(1):25-30.
[31]	HUANG M, YU J, HU Q, et al. Preparation and enhanced photocatalytic activity of carbon nitride/titania(001 vs 101 facets)/reduced graphene oxide (g-C3N4/TiO2/rGO) hybrids under visible light[J]. Appl. Surf. Sci., 2016, 389:1084-1093.
[32]	LAI C, WANG M M, ZENG G M, et al. Synthesis of surface molecular imprinted TiO2/graphene photocatalyst and its highly efficient photocatalytic degradation of target pollutant under visible light irradiation[J]. Appl. Surf. Sci., 2016, 390:368-376.
[33]	HU J, WANG L, ZHANG P, et al. Construction of solid-state Z-scheme carbon-modified TiO2/WO3 nanofibers with enhanced photocatalytic hydrogen production[J]. J. Power Sources, 2016, 328:28-36.
[34]	LI G, LIAN Z, WANG W, et al. Nanotube-confinement induced size-controllable g-C3N4, quantum dots modified single-crystalline TiO2, nanotube arrays for stable synergetic photoelectrocatalysis[J]. Nano Energy, 2016, 19:446-454.
[35]	JIN T, YAMAGUCHI T, TANABE K, et al. Infrared study of sulfur-containing iron oxide[J]. Inorg. Chem., 1984, 23:4396-4398.
[36]	JIN T, YAMAGUCHI T, TANABE K, et al. Structure of acid sites on sulfur-promoted iron oxide[J]. J. Phys. Chem., 1986, 90(14):31448-3152.
[37]	IUPAC. Manual of symbols and terminology[J]. Pure Appl. Chem., 1972, 31:578-638.
[38]	YANG R C, LU X J, ZHANG H, et al. Glycol-assisted construction of three-dimensionally ordered macroporous ZnO-Cu2O-TiO2 with enhanced photocatalytic properties[J]. Appl. Surf. Sci., 2016, 36:237-243.
[39]	LI Y, HWANG D S, LEE N H, et al. Synthesis and characterization of carbon-doped titania as an artificial solar light sensitive photocatalyst[J]. Chem. Phys. Lett., 2005, 404(1/2/3):25-29.
[40]	REN W, AI Z, JIA F, et al. Low temperature preparation and visible light photocatalytic activity of mesoporous carbon-doped crystalline TiO2[J]. Appl. Catal. B:Environ., 2007, 69(3):138-144.
[41]	GUAYAQUIL-SOSA J F, SERRANO-ROSALES B, et al. Photocatalytic hydrogen production using mesoporous TiO2 doped with Pt[J]. Appl. Catal. B:Environ., 2017, 211:337-348.):655-657.
[21]	彭少洪, 张渊明, 钟理. TiO2 基固体超强酸的制备及光催化性能研究[J]. 无机化学学报, 2006, 34(12):2258-2262. PENG S H, ZHANG Y M, ZHONG L. Preparation of TiO2-based solid superacid and its photocatalytic performance[J]. J. Inorg. Mater., 2006, 34(12):2258-2262.
[22]	YUAN H, HE J, LI R, et al. Characterization of SO42-/TiO2 and its catalytic activity in the epoxidation reaction[J]. Res. Chem. Intermed., 2017, 43:4353-4368.
[23]	MENG C, CAO G P, LI X K, et al. Structure of the SO42-/TiO2 solid acid catalyst and its catalytic activity in cellulose acetylation[J]. Reac. Kinet. Mech. Cat., 2017, 121:719-734.
[24]	VELMURUGAN R, KRISHNAKUMAR B, SWAMINATHAN M. Synthesis of Pd co-doped nanoTiO2-SO42-, and its synergetic effect on the solar photodegradation of Reactive Red 120 dye[J]. Mat. Sci. Semicon. Proc., 2014, 25(25):163-172.
[25]	FERNANDO K A, SAHU S, LIU Y, et al. Carbon quantum dots and applications in photocatalytic energy conversion.[J]. Acs Appl. Mater. Inter., 2015, 7(16):8363.
[26]	ZALFANI M, SCHUEREN B V D, MAHDOUANI M, et al. ZnO quantum dots decorated 3DOM TiO2, nanocomposites:Symbiose of quantum size effects and photonic structure for highly enhanced photocatalytic degradation of organic pollutants[J]. Appl. Catal. B:Environ., 2016, 199:187-198.
[27]	WANG X W, SUN G Z, LI N, et al. Quantum dots derived from two-dimensional materials and their applications for catalysis and energy[J]. Chem. Soc. Rev., 2016, 47(22):2239.
[28]	CHEN T, QUAN W, YU L, et al. One-step synthesis and visible-light-driven H2 production from water splitting of Ag quantum dots/g-C3N4 photocatalysts[J]. J. Alloy. Compd., 2016, 686:628-634.
[29]	Gutiérrez O Y, Pérez F, Fuentes G A, et al. Deep HDS over NiMo/Zr-SBA-15 catalysts with varying MoO3 loading[J]. Cataly. Today, 2008, 130(2-4):292-301.
[30]	YANG R C, ZHANG Z H, REN Y M, et al. Green synthesis of bi-component copper oxide composites and enhanced photocatalytic performance[J]. Mater. Sci. Tech-Lond., 2015, 31(1):25-30.
[31]	HUANG M, YU J, HU Q, et al. Preparation and enhanced photocatalytic activity of carbon nitride/titania(001 vs 101 facets)/reduced graphene oxide (g-C3N4/TiO2/rGO) hybrids under visible light[J]. Appl. Surf. Sci., 2016, 389:1084-1093.
[32]	LAI C, WANG M M, ZENG G M, et al. Synthesis of surface molecular imprinted TiO2/graphene photocatalyst and its highly efficient photocatalytic degradation of target pollutant under visible light irradiation[J]. Appl. Surf. Sci., 2016, 390:368-376.
[33]	HU J, WANG L, ZHANG P, et al. Construction of solidstate Z-scheme carbon-modified TiO2/WO3 nanofibers with enhanced photocatalytic hydrogen production[J]. J. Power Sources, 2016, 328:28-36.
[34]	LI G, LIAN Z, WANG W, et al. Nanotube-confinement induced size-controllable g-C3N4, quantum dots modified single-crystalline TiO2, nanotube arrays for stable synergetic photoelectrocatalysis[J]. Nano Energy, 2016, 19:446-454.
[35]	JIN T, YAMAGUCHI T, TANABE K,et al. Infrared study of sulfur-containing iron oxide[J]. Inorg. Chem., 1984, 23:4396-4398.
[36]	JIN T, YAMAGUCHI T, TANABE K, et al. Structure of acid sites on sulfur-promoted iron oxide[J]. J. Phys. Chem., 1986, 90(14):31448-3152.
[37]	IUPAC manual of symbols and terminology[J]. Pure Appl. Chem., 1972, 31:578-638.
[38]	YANG R C, LU X J, ZHANG H, et al. Glycol-assisted construction of three-dimensionally ordered macroporous ZnO-Cu2O-TiO2 with enhanced photocatalytic properties[J]. Appl. Surf. Sci., 2016, 36:237-243.
[39]	LI Y, HWANG D S, LEE N H, et al. Synthesis and characterization of carbon-doped titania as an artificial solar light sensitive photocatalyst[J]. Chem. Phys. Lett., 2005, 404(1-3):25-29.
[40]	REN W, AI Z, JIA F, et al. Low temperature preparation and visible light photocatalytic activity of mesoporous carbon-doped crystalline TiO2[J]. Appl. Catal. B:Environ., 2007, 69(3):138-144.
[41]	GUAYAQUIL-SOSA J F, SERRANO-ROSALES B, et al. Photocatalytic hydrogen production using mesoporous TiO2 doped with Pt[J]. Appl. Catal. B:Environ., 2017, 211:337-348.

C/TiO₂-SO₄^2-的制备及其光解水性能

Preparation of C/TiO₂-SO₄^2- and their water splitting performance

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献 41

相关文章 15

编辑推荐

Metrics

本文评价

[1]	黄琮琪, 吴一梅, 陈建业, 邵双全. 碱性电解水制氢装置热管理系统仿真研究[J]. 化工学报, 2023, 74(S1): 320-328.
[2]	李艺彤, 郭航, 陈浩, 叶芳. 催化剂非均匀分布的质子交换膜燃料电池操作条件研究[J]. 化工学报, 2023, 74(9): 3831-3840.
[3]	刘远超, 关斌, 钟建斌, 徐一帆, 蒋旭浩, 李耑. 单层XSe₂（X=Zr/Hf）的热电输运特性研究[J]. 化工学报, 2023, 74(9): 3968-3978.
[4]	杨学金, 杨金涛, 宁平, 王访, 宋晓双, 贾丽娟, 冯嘉予. 剧毒气体PH₃的干法净化技术研究进展[J]. 化工学报, 2023, 74(9): 3742-3755.
[5]	陈杰, 林永胜, 肖恺, 杨臣, 邱挺. 胆碱基碱性离子液体催化合成仲丁醇性能研究[J]. 化工学报, 2023, 74(9): 3716-3730.
[6]	胡兴枝, 张皓焱, 庄境坤, 范雨晴, 张开银, 向军. 嵌有超小CeO₂纳米粒子的碳纳米纤维的制备及其吸波性能[J]. 化工学报, 2023, 74(8): 3584-3596.
[7]	杨菲菲, 赵世熙, 周维, 倪中海. Sn掺杂的In₂O₃催化CO₂选择性加氢制甲醇[J]. 化工学报, 2023, 74(8): 3366-3374.
[8]	李凯旋, 谭伟, 张曼玉, 徐志豪, 王旭裕, 纪红兵. 富含零价钴活性位点的钴氮碳/活性炭设计及甲醛催化氧化应用研究[J]. 化工学报, 2023, 74(8): 3342-3352.
[9]	杨欣, 彭啸, 薛凯茹, 苏梦威, 吴燕. 分子印迹-TiO₂光电催化降解增溶PHE废水性能研究[J]. 化工学报, 2023, 74(8): 3564-3571.
[10]	陈佳起, 赵万玉, 姚睿充, 侯道林, 董社英. 开心果壳基碳点的合成及其对Q235碳钢的缓蚀行为研究[J]. 化工学报, 2023, 74(8): 3446-3456.
[11]	涂玉明, 邵高燕, 陈健杰, 刘凤, 田世超, 周智勇, 任钟旗. 钙基催化剂的设计合成及应用研究进展[J]. 化工学报, 2023, 74(7): 2717-2734.
[12]	张琦钰, 高利军, 苏宇航, 马晓博, 王翊丞, 张亚婷, 胡超. 碳基催化材料在电化学还原二氧化碳中的研究进展[J]. 化工学报, 2023, 74(7): 2753-2772.
[13]	邢美波, 张中天, 景栋梁, 张洪发. 磁调控水基碳纳米管协同多孔材料强化相变储/释能特性[J]. 化工学报, 2023, 74(7): 3093-3102.
[14]	余娅洁, 李静茹, 周树锋, 李清彪, 詹国武. 基于天然生物模板构建纳米材料及集成催化剂研究进展[J]. 化工学报, 2023, 74(7): 2735-2752.
[15]	葛加丽, 管图祥, 邱新民, 吴健, 沈丽明, 暴宁钟. 垂直多孔碳包覆的FeF₃正极的构筑及储锂性能研究[J]. 化工学报, 2023, 74(7): 3058-3067.