氧化石墨烯掺杂锌铝类水滑石负载钯金催化剂的制备及催化性能

doi:10.16085/j.issn.1000-6613.2017-0387

化工进展 ›› 2017, Vol. 36 ›› Issue (11): 4087-4092.DOI: 10.16085/j.issn.1000-6613.2017-0387

氧化石墨烯掺杂锌铝类水滑石负载钯金催化剂的制备及催化性能

马帅¹, 陈郑², 王家喜¹

1. 河北工业大学化工学院, 天津 300130;
2. 清华大学化学系, 北京 100084

收稿日期:2017-03-09 修回日期:2017-05-11 出版日期:2017-11-05 发布日期:2017-11-05
通讯作者: 王家喜,教授,主要从事金属有机催化方面研究。
作者简介:马帅(1990-),男,硕士研究生。E-mail:mashuaimail@126.com。

Preparation of GO doped Zn-Al LDHs supported palladium gold catalysts and their catalytic performances

MA Shuai¹, CHEN Zheng², WANG Jiaxi¹

1. Institute of Chemical Technology, Hebei University of Technology, Tianjin 300130, China;
2. Department of Chemistry, Tsinghua University, Beijing 100084, China

Received:2017-03-09 Revised:2017-05-11 Online:2017-11-05 Published:2017-11-05

摘要/Abstract

摘要： 采用离子交换-还原法制备了氧化石墨烯（GO）掺杂锌铝类水滑石负载钯金双金属纳米颗粒的催化剂（PdAu/Zn-Al LDHs/GO），通过XRD、TEM表征了催化剂的结构，以GO掺杂锌铝类水滑石为载体负载钯金纳米颗粒粒径小（约2nm）且分散均匀。以苯甲醇空气氧化形成苯甲醛的反应为模型，评价催化剂的催化性能，探讨了载体及钯、金比例对催化反应的影响。催化结果表明，氧化石墨烯掺杂的锌铝类水滑石是考察载体中最好的钯、金催化剂的载体，随着钯金比的增加催化剂的催化活性先增加后降低，生成苯甲醛的选择性下降，当钯金比例为1：1时，催化剂（Pd₁Au₁/Zn-Al LDHs/GO）的综合催化性能最好，催化活性随反应温度的升高而升高，但选择性随温度的升高而下降。在Pd₁Au₁/Zn-Al LDHs/GO催化下，80℃反应8h后苯甲醇的转化率可达96%，苯甲醛的选择性为93%，催化剂循环使用4次后仍保持较好的催化性能。

关键词: 醇, 氧化, 纳米粒子, 水滑石, 氧化石墨烯

Abstract: Palladium-gold bimetallic nanoparticles deposited on the graphene oxide(GO)doped Zn-Al layered double hydroxide(PdAu/Zn-Al LDHs/GO)were synthesized through the ion exchange-reduction method. The as-prepared supported palladium-gold bimetallic catalysts were characterized by XRD and TEM. The bimetallic nanoparticles loaded by the GO doped Zn-Al LDHs as the carrier is uniform and the particle size is about 2nm. The catalytic activities of as-prepared catalysts were evaluated by using oxidation of benzyl alcohol to benzaldehyde as the model reaction. The effects of carriers and ratio of Pd/Au on the catalytic properties were investigated. The catalytic results showed that the LDHs/GO was the best among the used carriers. As the increase of ratio of Pd/Au,the activity of supported catalyst increased at first,and then decreased,whereas the selectivity of benzaldehyde decreased. With the ratio of Pd/Au being 1:1 at 80℃,the performances of Pd₁Au₁/Zn-Al LDHs/GO is the best. The catalytic activity increased as the increase of temperature,but the selectivity of benzaldehyde decreased. Under promotion of Pd₁Au₁/Zn-Al LDHs/GO at 80℃ for 8h,the conversion of benzyl alcohol and selectivity of benzaldehyde was 96% and 93%,respectively. The catalyst of Pd₁Au₁/Zn-Al LDHs/GO still maintained excellent catalytic performance after four cycles.

Key words: alcohols, oxidation, nanoparticles, layered double hydroxide, graphene oxide

中图分类号:

O643.3

马帅, 陈郑, 王家喜. 氧化石墨烯掺杂锌铝类水滑石负载钯金催化剂的制备及催化性能[J]. 化工进展, 2017, 36(11): 4087-4092.

MA Shuai, CHEN Zheng, WANG Jiaxi. Preparation of GO doped Zn-Al LDHs supported palladium gold catalysts and their catalytic performances[J]. Chemical Industry and Engineering Progress, 2017, 36(11): 4087-4092.

参考文献

[1] 刘向文,王定胜,彭卿,等.双金属纳米材料与催化[J]. 中国科学:化学,2014,44(1):85-99. LIU X W,WANG D S,PENG Q,et al.Bimetal catalytic nanomaterials[J].Science China:Chemistry,2014,44(1):85-99.
[2] TEIXEIRA-NETO A A,FACETO B,SIEBRA L S,et al.Effect of the synthesis method on the properties and catalytic activities of Au/Pd nanoparticles supported on organophilic clay[J].Applied Clay Science,2015,116:175-181.
[3] FANG W,DENG Y,TANG L,et al.Synthesis of Pd/Au bimetallic nanoparticle-loaded ultrathin graphitic carbon nitride nanosheets for highly efficient catalytic reduction of p-nitrophenol[J].Journal of Colloid and Interface Science,2017,490:834-843.
[4] CHEN Z,WANG S,LIAN C,et al.Nano PdAu bimetallic alloy as an effective catalyst for the Buchwald-Hartwig reaction[J]. Chemistry:An Asian Journal,2016,11(3):351-355.
[5] FERRAZ C P,GARCIA M A S,TEIXEIRA-NETO É,et al.Oxidation of benzyl alcohol catalyzed by gold nanoparticles under alkaline conditions:weak vs.strong bases[J].RSC Advances,2016,6(30):25279-25285.
[6] ALAYOGLU S,NILEKAR A U,MAVRIKAKIS M,et al.Ru-Pt core-shell nanoparticles for preferential oxidation of carbon monoxide in hydrogen[J].Nature Materials,2008,7(4):333-338.
[7] FANG W,ZHANG Q,CHEN J,et al.Gold nanoparticles on hydrotalcites as efficient catalysts for oxidant-free dehydrogenation of alcohols[J].Chemical Communications,2010,46(9):1547-1549.
[8] 郑建华,刘鹏,庞海霞.类水滑石在有机液相氧化中的催化应用[J]. 化工进展,2003,22(8):823-827. ZHENG J H,LIU P,PANG H X.Catalytic application of hydrotalcite-like compounds in liquid phase oxidation[J].Chemical Industry and Engineering Progress,2003,22(8):823-827.
[9] 李冰杰,史秀锋,刘秀芳,等.ZnAl水滑石负载钯催化剂的制备及催化性能[J].化工进展,2014,33(10):2661-2664. LI B J,SHI X F,LIU X F,et al.Preparation of hydrotalcite-supported palladium catalysts and their catalytic performances[J].Chemical Industry and Engineering Progress,2014,33(10):2661-2664.
[10] SUN J,HAN Y,FU H,et al.Au@Pd/TiO₂ with atomically dispersed Pd as highly active catalyst for solvent-free aerobic oxidation of benzyl alcohol[J]. Chemical Engineering Journal,2017,313:1-9.
[11] MITSUDOME T,NOUJIMA A,MIZUGAKI T,et al.Efficient aerobic oxidation of alcohols using a hydrotalcite-supported gold nanoparticle catalyst[J].Advanced Synthesis & Catalysis,2009,351(11/12):1890-1896.
[12] DU Y,WANG Q,LIANG X,et al.Hydrotalcite-like MgMnTi non-precious-metal catalyst for solvent-free selective oxidation of alcohols[J].Journal of Catalysis,2015,331:154-161.
[13] EIGLER S,HIRSH A.Chemistry with graphene and graphene oxide-challenges for synthetic chemists[J].Angewandte Chemie International Edition,2014,53(30):7720-7738.
[14] SHANG N,FENG C,ZHANG H,et al.Suzuki-Miyaura reaction catalyzed by graphene oxide supported palladium nanoparticles[J].Catalysis Communications,2013,40:111-115.
[15] 肖淑娟,于守武,谭小耀.石墨烯类材料的应用及研究进展[J].化工进展,2015,34(5):1345-1348. XIAO S J,YU S W,TAN X Y.Research progress and the applications of graphene materials[J].Chemical Industry and Engineering Progress,2015,34(5):1345-1348.
[16] HATUI G,NAYAK G C,UDAYABHANU G.One pot solvothermal synthesis of sandwich-like Mg Al layered double hydroxide anchored reduced graphene oxide:an excellent electrode material for supercapacitor[J]. Electrochimica Acta,2016,219:214-226.
[17] AHMED N S,MENZEL R,WANG Y,et al. Graphene-oxide-supported CuAl and CoAl layered double hydroxides as enhanced catalysts for carbon-carbon coupling via Ullmann reaction[J]. Journal of Solid State Chemistry,2017,246:130-137.
[18] 吴鑫干,尹娟娟,胡在君.苯甲醛的合成进展[J].精细石油化工,2002(4):57-63. WU X G,YIN J J,HU Z J.Progress in benzaldehyde synthesis[J].Speciality Petrochemicals,2002(4):57-63.
[19] 朱宪,王彬,张彰,等.苯甲醛清洁生产工艺技术研究进展[J].化工进展,2005,24(2):109-116. SONG X,WANG B,ZHANG Z,et al. Progress of cleaner technology for benzaldehyde synthesis[J].Chemical Industry and Engineering Progress,2005,24(2):109-116.
[20] MALLAT T,BAIKER A.Oxidation of alcohols with molecular oxygen on solid catalysts[J].Chemical Reviews,2004,104(6):3037-3058.
[21] 万臣,彭同江,孙红娟,等.不同氧化程度氧化石墨烯的制备及湿敏性能研究[J].无机化学学报,2012,28(5):915-921. WAN C,PENG T J,SUN H J,et al.Preparation and humidity-sensitive properties of graphene oxide in different oxidation degree[J].Chinese Journal of Inorganic Chemistry,2012,28(5):915-921.
[22] 刘芳,朱文凤,王林江,等.温和条件下硝酸根型ZnAl-LDHs的合成与表征[J].武汉理工大学学报,2012,34(1):12-15. LIU F,ZHU W F,WANG L J,et al.The preparation and characterization of ZnAl-LDHs at mild pH value[J].Journal of Wuhan University of Technology,2012,34(1):12-15.
[23] ZHAO M Q,ZHANG Q,ZHANG W,et al.Embedded high density metal nanoparticles with extraordinary thermal stability derived from guest-host mediated layered double hydroxides[J].Journal of the American Chemical Society,2010,132(42):14739-14741.

氧化石墨烯掺杂锌铝类水滑石负载钯金催化剂的制备及催化性能

Preparation of GO doped Zn-Al LDHs supported palladium gold catalysts and their catalytic performances

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	张明焱, 刘燕, 张雪婷, 刘亚科, 李从举, 张秀玲. 非贵金属双功能催化剂在锌空气电池研究进展[J]. 化工进展, 2023, 42(S1): 276-286.
[2]	时永兴, 林刚, 孙晓航, 蒋韦庚, 乔大伟, 颜彬航. 二氧化碳加氢制甲醇过程中铜基催化剂活性位点研究进展[J]. 化工进展, 2023, 42(S1): 287-298.
[3]	谢璐垚, 陈崧哲, 王来军, 张平. 用于SO₂去极化电解制氢的铂基催化剂[J]. 化工进展, 2023, 42(S1): 299-309.
[4]	杨霞珍, 彭伊凡, 刘化章, 霍超. 熔铁催化剂活性相的调控及其费托反应性能[J]. 化工进展, 2023, 42(S1): 310-318.
[5]	郑谦, 官修帅, 靳山彪, 张长明, 张小超. 铈锆固溶体Ce_0.25Zr_0.75O₂光热协同催化CO₂与甲醇合成DMC[J]. 化工进展, 2023, 42(S1): 319-327.
[6]	戴欢涛, 曹苓玉, 游新秀, 徐浩亮, 汪涛, 项玮, 张学杨. 木质素浸渍柚子皮生物炭吸附CO₂特性[J]. 化工进展, 2023, 42(S1): 356-363.
[7]	张祚群, 高扬, 白超杰, 薛立新. 二次界面聚合同步反扩散原位生长ZIF-8纳米粒子制备聚酰胺混合基质反渗透（RO）膜[J]. 化工进展, 2023, 42(S1): 364-373.
[8]	王正坤, 黎四芳. 双子表面活性剂癸炔二醇的绿色合成[J]. 化工进展, 2023, 42(S1): 400-410.
[9]	许家珩, 李永胜, 罗春欢, 苏庆泉. 甲醇水蒸气重整工艺的优化[J]. 化工进展, 2023, 42(S1): 41-46.
[10]	高雨飞, 鲁金凤. 非均相催化臭氧氧化作用机理研究进展[J]. 化工进展, 2023, 42(S1): 430-438.
[11]	顾永正, 张永生. HBr改性飞灰对Hg⁰的动态吸附及动力学模型[J]. 化工进展, 2023, 42(S1): 498-509.
[12]	孙玉玉, 蔡鑫磊, 汤吉海, 黄晶晶, 黄益平, 刘杰. 反应精馏合成甲基丙烯酸甲酯工艺优化及节能[J]. 化工进展, 2023, 42(S1): 56-63.
[13]	李梦圆, 郭凡, 李群生. 聚乙烯醇生产中回收工段第三、第四精馏塔的模拟与优化[J]. 化工进展, 2023, 42(S1): 113-123.
[14]	盛维武, 程永攀, 陈强, 李小婷, 魏嘉, 李琳鸽, 陈险峰. 微气泡和微液滴双强化脱硫反应器操作分析[J]. 化工进展, 2023, 42(S1): 142-147.
[15]	赵晨, 苗天泽, 张朝阳, 洪芳军, 汪大海. 负压状态窄缝通道乙二醇水溶液传热特性[J]. 化工进展, 2023, 42(S1): 148-157.