贵金属催化剂理性设计在选择性加氢反应中的研究进展

doi:10.19964/j.issn.1006-4990.2021-0008

摘要/Abstract

摘要：

从多相催化的特征出发,综述了多相催化理性设计中典型调控理论和方法的研究进展。同时,以芳香硝基化合物及不饱和醛/酮选择性加氢反应为特征反应,从多相催化剂表面的电子效应、几何效应、界面效应和协同效应等角度进行了全面综述。指出了筛选合适的载体、合成特定尺寸形貌的活性中心、调控金属-载体强相互作用是开发更高效的多相选择性加氢催化剂的重要方向,调控金属-载体强相互作用,优化活性中心的电子效应、空间效应和界面效应,微调N=O及C=O不饱和键的吸附与活化,是实现高效选择性加氢催化体系的理论设计的重要手段。进一步优化氢气的活化裂解方式、活性氢的稳定与迁移,可抑制选择性加氢的副反应。

关键词: 贵金属催化剂, 多相催化, 选择性加氢, 理性设计

Abstract:

Based on the characteristics of heterogeneous catalysis,the research progress of typical regulatory theories and methods in the rational design of heterogeneous catalysis was reviewed.Meanwhile,from the perspectives of electronic effects,geometric effects,interfacial effects and synergetic effects,the relationship between surface structure of active centers and selective hydrogenation performance was reviewed comprehensively,with selective hydrogenation of aromatic nitro compounds and unsaturated aldehydes/ketones as a probe reaction.It was pointed out that selecting suitable supports,synthesizing metal active centers with specific size and morphology,and regulating the strong metal-support interaction were effective ways to regulate the performance of selective hydrogenation catalysts.The adsorption and activation of N=O and C=O could be precisely tuned by optimizing the electronic effect,spatial effect and interface effect of active center resulted from the strong metal-support interaction,which was important to the rational design of efficient selective hydrogenation catalysts.Further optimization of hydrogen activation cracking mode,stability and migration of active hydrogen could inhibit the side reaction of selective hydrogenation.

Key words: noble catalysts, heterogeneous catalysis, selective hydrogenation, rational design

中图分类号:

O643.36

马明超,臧甲忠,于海斌,范景新,郭春垒,靳凤英. 贵金属催化剂理性设计在选择性加氢反应中的研究进展[J]. 无机盐工业, 2021, 53(7): 23-29.

Ma Mingchao,Zang Jiazhong,Yu Haibin,Fan Jingxin,Guo Chunlei,Jin Fengying. Research progress rational design of noble metal catalysts for selective hydrogenation[J]. Inorganic Chemicals Industry, 2021, 53(7): 23-29.

图/表 3

参考文献 59

[1]	Liu L C, Corma A. Metal catalysts for heterogeneous catalysis:From single atoms to nanoclusters and nanoparticles[J]. Chemical Revie-ws, 2018, 118(10):4981-5079.
[2]	Somorjai G A, Yang M. The surface science of catalytic selectivi-ty[J]. Topics in Catalysis, 2003, 24(1):61-72.
[3]	Gertl H K, Knözinger H. Handbook of heterogeneous catalysis[M]. New York:Wiley-VCH, 1997:46-48.
[4]	朱利安R.H.罗斯. 多相催化:基本原理与应用[M]. 田野,张立红,赵宜成,等译. 北京: 化学工业出版社, 2016.
[5]	Somorjai G A, Park J Y. Molecular factors of catalytic selectivity[J]. Angewandte Chemie International Edition, 2008, 47:9212-9228.
[6]	Zhang S, Chang C R, Huang Z Q, et al. High catalytic activity and chemoselectivity of sub-nanometric Pd clusters on porous nanorods of CeO₂ for hydrogenation of nitroarenes[J]. Journal of the American Chemical Society, 2016, 138(8):2629-2637.
[7]	Wu B, Zheng N F. Surface and interface control of noble metal nanocrystals for catalytic and electrocatalytic applications[J]. Nano Today, 2013, 8:168-197.
[8]	Ye T N, Xiao Z, Li J, et al. Stable single platinum atoms trapped in sub-nanometer cavities in 12CaO·7Al₂O₃ for chemoselective hydro-genation of nitroarenes[J]. Nature Communications, 2020, 11.Doi: 10.1038/s41467-019-14216-9.
[9]	Serna P, Boronat M, Corma A. Tuning the behavior of Au and Pt cat- alysts for the chemoselective hydrogenation of nitroaromatic compo-unds[J]. Topics in Catalysis, 2011, 54(5/6/7):439-446.
[10]	Corma A, Serna P, Concepción P, et al. Transforming nonselective into chemoselective metal catalysts for the hydrogenation of sub- stituted nitroaromatics[J]. Journal of the American Chemical So-ciety, 2008, 130(27):8748-8753.
[11]	Huang W, Sun G, Cao T. Surface chemistry of group IB metals and related oxides[J]. Chemical Society Reviews, 2017, 46:1977-2000.
[12]	Zhao M, Yuan K, Wang Y, et al. Metal-organic frameworks as se-lectivity regulators for hydrogenation reactions[J]. Nature, 2016, 539:76-80.
[13]	Lu J, Low K B, Lei Y, et al. Toward atomically-precise synjournal of supported bimetallic nanoparticles using atomic layer deposi-tion[J]. Nature Communications, 2014, 5.Doi: 10.1038/ncomms4264.
[14]	Nϕrskov J K, Bligaard T, Rossmeisl J, et al. Towards the computational design of solid catalysts[J]. Nature Chemistry, 2009, 1(1):37-46.
[15]	Noyori R. Synthesizing our future[J]. Nature Chemistry, 2009, 1(1):5-6.
[16]	Ertl G. Heterogeneous catalysis on the atomic scale[J]. The Chemi-cal Record, 2001, 1(1):33-45.
[17]	Boudart M. Heterogeneous catalysis by metals[J]. Journal of Molec-ular Catalysis, 1985, 30:27-38.
[18]	Boudart M. Catalysis by supported metals[J]. Advances in Cataly-sis, 1969, 20:153-166.
[19]	Boronat M, Leyva-Pérez A, Corma A. Theoretical and experimental insights into the origin of the catalytic activity of subnanometric gold clusters:Attempts to predict reactivity with clusters and nano-particles of gold[J]. Accounts of Chemical Research, 2014, 47(3):834-844.
[20]	Gerhard E. Heterogeneous catalysis on atomic scale[J]. Journal of Molecular Catalysis A:Chemical, 2002, 182/183:5-16.
[21]	Chen G, Xu C, Huang X, et al. Interfacial electronic effects control the reaction selectivity of platinum catalysts[J]. Nature Materials, 2016, 15:564-569.
[22]	Novotny Z, Argentero G, Wang Z M, et al. Ordered array of single Au adatoms with remarkable thermal stability:Au/Fe₃O₄(001)[J]. Physical Review Letters, 2012, 108.Doi: 10.1103/PhysRevLett.108.216103.
[23]	Ferguson G A, Yin C R, Kwon G, et al. Stable subnanometer cobalt oxide clusters on ultrananocrystalline diamond and alumina supports:Oxidation state and the origin of sintering resistance[J]. The Journal of Physical Chemistry C, 2012, 116(45):24027-24034.
[24]	Bell A T. The impact of nanoscience on heterogeneous catalysis[J]. Science, 2003, 299:1688-1691.
[25]	Chen M S, Goodman D W. The structure of catalytically active gold on titania[J]. Science, 2004, 306:252-255.
[26]	Hansen T W, DeLaRiva A T, Challa S R, et al. Sintering of catalytic nanoparticles:Particle migration or Ostwald ripening?[J]. Accounts of Chemical Research, 2013, 46(8):1720-1730.
[27]	Sanchez S I, Menard L D, Bram A, et al. The emergence of nonbulk properties in supported metal clusters:Negative thermal expansion and atomic disorder in Pt nanoclusters supported on γ-Al₂O₃[J]. Journal of the American Chemical Society, 2009, 131(20):7040-7054.
[28]	Yang X F, Wang A Q, Qiao B T, et al. Single-atom catalysts:A new frontier in heterogeneous catalysis[J]. Accounts of Chemical Re-search, 2013, 46(8):1740-1748.
[29]	Bao X H. Fundamental research in catalysis with emphasis on con-finement effects[J]. Scientia Sinica Chimica, 2012, 42(4).Doi: 10.1360/032012-130.
[30]	Li H, Xiao J, Fu Q, et al. Confined catalysis under two-dimensional materials[J]. Proceedings of the National Academy of Sciences of the United States of America, 2017, 114:5930-5934.
[31]	Dejong K P, Zecevic J. The platinum tush[J]. Nature Materials, 2017, 16:7-8.
[32]	Corma A, Serna P. Chemoselective hydrogenation of nitro compoun-ds with supported gold catalysts[J]. Science, 2006, 313:332-334.
[33]	Bhogeswararao S, Srinivas D. Intramolecular selective hydrogena-tion of cinnamaldehyde over CeO₂-ZrO₂ supported Pt catalysts[J]. Journal of Catalysis, 2012, 285:31-40.
[34]	Shi W, Zhang B S, Lin Y M, et al. Enhanced chemoselective hydro-genation through tuning the interaction between Pt nanoparticles and carbon supports:Insights from identical location transmission electron microscopy and X-ray photoelectron spectroscopy[J]. ACS Catalysis, 2016, 6(11):7844-7854.
[35]	Pan H, Li J, Lu J, et al. Selective hydrogenation of cinnamaldehyde with PtFeO_x/Al₂O₃@SBA-15 catalyst:Enhancement in activity and selectivity to unsaturated alcohol by Pt-FeO_x and Pt-Al₂O₃@SBA-15 interaction[J]. Journal of Catalysis, 2017, 354:24-36.
[36]	Shu Y, Chan H C, Xie L, et al. Bimetallic platinum-tin nanoparti-cles on hydrogenated molybdenum oxide for the selective hydro-genation of functionalized nitroarenes[J]. ChemCatChem, 2017, 9:4199-4205.
[37]	Wang A, Li J, Zhang T. Heterogeneous single-atom catalysis[J]. Nature Reviews Chemistry, 2018(2):65-81.
[38]	Wang C P, Mao S J, Wang Z, et al. Insight into single-atom-induced unconventional size dependence over CeO₂-supported Pt catalys-ts[J]. Chem, 2020, 6(3):752-765.
[39]	Wei H, Liu X, Wang A, et al. FeO_x-supported platinum single-atom and pseudo-single-atom catalysts for chemoselective hydrogena-tion of functionalized nitroarenes[J]. Nature Communications, 2014, 5.Doi: 10.1038/ncomms6634.
[40]	Feng H, Lu J L, Stair P C, et al. Alumina over-coating on Pd nano-particle catalysts by atomic layer deposition:Enhanced stability and reactivity[J]. Catalysis Letters, 2011, 141(4):512-517.
[41]	Hu Q, Wang S, Gao Z, et al. The precise decoration of Pt nanopar-ticles with Fe oxide by atomic layer deposition for the selective hydrogenation of cinnamaldehyde[J]. Applied Catalysis B:Enviro-nmental, 2017, 218:591-599.
[42]	He T W, Zhang C M, Zhang L, et al. Single Pt atom decorated graphitic carbon nitride as an efficient photocatalyst for the hydrogenation of nitrobenzene into aniline[J]. Nano Research, 2019, 12(8):1817-1823.
[43]	Cárdenas Lizana F, Hao Y F, Crespo Quesada M, et al. Selective gas phase hydrogenation of p-chloronitrobenzene over Pd catalysts:Role of the support[J]. ACS Catalysis, 2013, 3(6):1386-1396.
[44]	Mao S J, Zhao B W, Wang Z, et al. Tuning the catalytic performance for the semi-hydrogenation of alkynols by selectively poisoning the active sites of Pd catalysts[J]. Green Chemistry, 2019, 21:4143-4151.
[45]	曾昭槐. 择形催化[M]. 北京: 中国石化出版社, 1994:145-153.
[46]	Zhang J, Wang L, Shao Y, et al. A Pd@zeolite catalyst for nitroarene arene hydrogenation with high product selectivity by sterically controlled adsorption in the zeolite micropores[J]. Angewandte Chemie International Edition, 2017, 56:9747-9751.
[47]	Guo Z Y, Xiao C X, Maligal Ganesh R V, et al. Pt nanoclusters confined within metal-organic framework cavities for chemoselec-tive cinnamaldehyde hydrogenation[J]. ACS Catalysis, 2014, 4(5):1340-1348.
[48]	Li X F, Wang Z, Mao S J, et al. Insight into the role of additives in catalytic synjournal of cyclohexylamine from nitrobenzene[J]. Chinese Journal of Catalysis, 2018, 36:1191-1196.
[49]	Chen Y Z, Kong X Q, Mao S J, et al. Study on the role of alkaline sodium additive in selective hydrogenation of phenol[J]. Chinese Journal of Catalysis, 2019, 40:1516-1524.
[50]	Mao S J, Wang C P, Wang Y, et al. The chemical nature of N doping on N doped carbon supported noble metal catalysts[J]. Journal of Catalysis, 2019, 375:456-465.
[51]	Chen Y Z, Wang Z, Mao S J, et al. Rational design of hydrogenation catalysts using nitrogen-doped porous carbon[J]. Chinese Journal of Catalysis, 2019, 40:971-979.
[52]	Liu J R, Xie L, Wang Z, et al. Biomass-derived ordered mesoporous carbon nano-ellipsoid encapsulated metal nanoparticles inside:Ideal nanoreactors for shape-selective catalysis[J]. Chemical Communications, 2020, 56(2):229-232.
[53]	Jing P, Gan T, Qi H, et al. Synergism of Pt nanoparticles and iron oxide support for chemoselective hydrogenation of nitroarenes un-der mild conditions[J]. Chinese Journal of Catalysis, 2019, 40:214-222.
[54]	Serna P, Concepción P, Corma A. Design of highly active and che-moselective bimetallic gold-platinum hydrogenation catalysts thr-ough kinetic and isotopic studies[J]. Journal of Catalysis, 2009, 265:19-25.
[55]	Chandler B D. An extra layer of complexity[J]. Nature Chemistry, 2017, 9:108-109.
[56]	Dandekar A, Vannice M A. Crotonaldehyde hydrogenation on Pt/TiO₂ and Ni/TiO₂ SMSI catalysts[J]. Journal of Catalysis, 1999, 183:344-354.
[57]	Concepción P, Corma A, Silvestre Albero J, et al. Chemoselective hydrogenation catalysts:Pt on mesostructured CeO₂ nanoparticles embedded within ultrathin layers of SiO₂ binder[J]. Journal of the American Chemical Society, 2004, 126(17):5523-5532.
[58]	Kennedy G, Baker L R, Somorjai G A. Selective amplification of CO bond hydrogenation on Pt/TiO₂:Catalytic reaction and sum-frequ-ency generation vibrational spectroscopy studies of crotonaldehyde hydrogenation[J]. Angewandte Chemie International Edition, 2014, 53:3405-3408.
[59]	Kennedy G, Melaet G, Han H L, et al. In situ spectroscopic investi-gation into the active sites for crotonaldehyde hydrogenation at the Pt nanoparticle-Co₃O₄ interface[J]. ACS Catalysis, 2016, 6(10):7140-7147.

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