Computational exploration on effects of heteroatom doping for nanostructured carbon catalysts

doi:10.3969/j.issn.0438-1157.2014.07.025

Abstract

Abstract: Nanostructured carbon materials have become an important class of non-metal catalysts. One of the effective ways to tailor the properties of nanostructured carbon catalysts is heteroatoms doping. In the current study, three cases were selected to demonstrate the effects of heteroatoms doping with boron or nitrogen. They were partial oxidation of methane, selectivity in oxidative dehydrogenation reaction, and halogenation of acetylene. Computational studies revealed that doping did enhance the catalytic capabilities of nanostructured carbon catalysts. Moreover it could modulate the electronic structure and acid/base properties of the catalysts. The reaction mechanism was different from metal catalyst. Overall, the current study is crucial for the further development of nanostructured carbon catalysts and sheds light on the new strategy for optimization of catalytic performance.

Key words: computational chemistry, partial oxidation, catalyst activation, nanostructured carbon material, heteroatom

摘要： 纳米碳材料已经成为一类重要的非金属催化剂。通过在纳米碳材料催化剂中引入杂原子可以有效地改变催化剂的性能。通过3个研究实例分别说明了杂原子硼和氮在甲烷部分氧化、氧化脱氢反应中乙烯选择性和乙炔卤化反应中的作用和机理。通过研究表明硼和氮杂原子可以优化纳米碳材料的催化效果，改变催化剂的电子结构和酸碱性，揭示了碳材料与金属催化剂的不同作用机理。当前计算结果可为进一步提高纳米碳材料催化剂催化能力奠定基础。

关键词: 计算化学, 部分氧化, 催化剂活化, 纳米碳材料, 杂原子

CLC Number:

O643.3

LI Bo, SU Dangsheng. Computational exploration on effects of heteroatom doping for nanostructured carbon catalysts[J]. CIESC Journal, 2014, 65(7): 2657-2667.

李波, 苏党生. 利用杂原子调控纳米碳材料催化剂催化能力的初步探索[J]. 化工学报, 2014, 65(7): 2657-2667.

References 46

[1]	Serp P, Figueiredo J L. Carbon Materials for Catalysis[M]. Hoboken: Wiley, 2009
[2]	Machado B F, Serp P. Graphene-based materials for catalysis[J]. Catal. Sci. Technol., 2012, 2: 54-75
[3]	Zhu J, Holmen A, Chen D. Carbon nanomaterials in catalysis: proton affinity, chemical and electronic properties, and their catalytic consequences[J]. ChemCatChem, 2013, 5: 378-401
[4]	Figueiredo J L, Pereira M F R. The role of surface chemistry in catalysis with carbons[J]. Catal. Today, 2010, 150: 2-7
[5]	Su D S, Perathoner S, Centi G. Nanocarbons for the development of advanced catalysts[J]. Chem. Rev., 2013, 113: 5782-5816
[6]	Bitter J H. Nanostructured carbons in catalysis a Janus material-industrial applicability and fundamental insights[J]. J. Mater. Chem., 2010, 20: 7312-7321
[7]	Su D S, Zhang J, Frank B, Thomas A, Wang X, Paraknowitsch J, Schlögl R. Metal-free heterogeneous catalysis for sustainable chemistry[J]. ChemSusChem, 2010, 3: 169-180
[8]	Yu D, Nagelli E, Du F, Dai L. Metal-free carbon nanomaterials become more active than metal catalysts and last longer[J]. J. Phys. Chem. Lett., 2010, 1: 2165-2173
[9]	Zhang J, Liu X, Blume R, Zhang A, Schlögl R, Su D S. Surface-modified carbon nanotubes catalyze oxidative dehydrogenation of n-butane[J]. Science, 2008, 322: 73-77
[10]	Wang H, Maiyalagan T, Wang X. Review on recent progress in nitrogen-doped graphene: synthesis, characterization, and its potential applications[J]. ACS Catalysis, 2012, 2: 781-794
[11]	Liu H T, Liu Y Q, Zhu D B. Chemical doping of graphene[J]. J. Mater. Chem., 2011, 21: 3335-3345
[12]	Ewels C P, Glerup M. Nitrogen doping in carbon nanotubes[J]. J. Nanosci. Nanotech., 2005, 5: 1345-1363
[13]	Ayala P, Arenal R, Rümmeli M, Rubio A, Pichler T. The doping of carbon nanotubes with nitrogen and their potential applications[J]. Carbon, 2010, 48: 575-586
[14]	Gong K, Du F, Xia Z, Durstock M, Dai L, Nitrogen-doped carbon nanotube arrays with high electrocatalytic activity for oxygen reduction[J]. Science, 2009, 323: 760-764
[15]	Liang J, Jiao Y, Jaroniec M, Qiao S Z. Sulfur and nitrogen dual-doped mesoporous graphene electrocatalyst for oxygen reduction with synergistically enhanced performance[J]. Angew. Chem. Int. Ed., 2012, 51: 11496-11500
[16]	Yu S, Zheng W, Wang C, Jiang Q. Nitrogen/boron doping position dependence of the electronic properties of a triangular graphene[J]. ACS Nano, 2010, 4: 7619-7629
[17]	Zhao Y, Yang L J, Chen S, Wang X Z, Ma Y W, Wu Q, Jiang Y F, Qian W J, Hu Z. Can boron and nitrogen co-doping improve oxygen reduction reaction activity of carbon nanotubes? [J]. J. Am. Chem. Soc., 2013, 135: 1201-1204
[18]	Talla J A. First principles modeling of boron-doped carbon nanotube sensors[J]. Phys. B: Condes. Matt., 2012, 407: 966-970
[19]	Cao Y H, Yu H, Tan J, Peng F, Wang H J, Li J, Zheng W X, Wong N B. Nitrogen-, phosphorous- and boron-doped carbon nanotubes as catalysts for the aerobic oxidation of cyclohexane[J]. Carbon, 2013, 57: 433-442
[20]	Schwartz V, Xie H, Meyer H M, Overbury S H, Liang C D. Oxidative dehydrogenation of isobutane on phosphorous-modified graphitic mesoporous carbon[J]. Carbon, 2011, 49: 659-668
[21]	Christian E B, Lødeng R, Holmen A. A review of catalytic partial oxidation of methane to synthesis gas with emphasis on reaction mechanisms over transition metal catalysts[J]. Appl. Catal. A, 2008, 346: 1-27
[22]	Fierro J L G. Catalysis in C1 chemistry — future and prospect[J]. Catal. Lett., 1993, 22: 67-91
[23]	Alvarez-Galvan M C, Mota N, Ojeda M, Rojas S, Navarro R M, Fierro J L G. Direct methane conversion routes to chemicals and fuels[J]. Catal. Today, 2011, 171: 15-23
[24]	Li B, Su D S. First-principles studies of the activation of oxygen molecule and its role in partial oxidation of methane on boron-doped single-walled carbon nanotubes[J]. J. Phys. Chem. C, 2013, 117: 17485-17492
[25]	Grabowski R. Kinetics of oxidative dehydrogenation of C2—C3 alkanes on oxide catalysts[J]. Catal. Rev. Sci. Eng., 2006, 48: 199-268
[26]	Kung H H. Oxidative dehydrogenation of light (C2 to C6) alkanes[J]. Adv. Catal., 1994, 40: 1-38
[27]	Kresse G, Joubert D. From ultrasoft pseudopotentials to the projector augmented-wave method[J]. Phys. Rev. B, 1999, 59: 1758
[28]	Perdew J P, Burke K, Ernzerhof M. Generalized gradient approximation made simple[J]. Phys. Rev. Lett., 1996, 77: 3865-3868
[29]	Henkelman G, Uberuaga B P, Jonsson H. A climbing image nudged elastic band method for finding saddle points and minimum energy paths[J]. J. Chem. Phys., 2000, 113: 9901-9904
[30]	Kresse G, Furthmüller J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set[J]. Comput. Matt. Sci., 1996, 6: 15-50
[31]	Kresse G, Furthmüller J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set[J]. Phys. Rev. B, 1996, 54: 11169
[32]	Savin A, Becke A D, Flad J, Nesper R, Preuss H, von Schnering H G. A new look at electron localization[J]. Angew. Chem. Int. Ed., 1991, 30: 409-412
[33]	Tang W, Hu Z P, Wang M J, Stucky G D, Metiu H, McFarland E W. Methane complete and partial oxidation catalyzed by Pt-doped CeO2[J]. J. Catal., 2010, 273: 125-137
[34]	Hu X, Zhou Z, Lin Q, Wu Y, Zhang Z. High reactivity of metal-free nitrogen-doped carbon nanotube for the C—H activation[J]. Chem. Phys. Lett., 2011, 503: 287-291
[35]	Frank B, Zhang J, Blume R, Schlögl R, Su D. Heteroatoms increase the selectivity in oxidative dehydrogenation reactions on nanocarbons[J]. Angew. Chem. Int. Ed., 2009, 48: 6913-6917
[36]	Li B, Su D. Theoretical studies on ethylene selectivity in the oxidative dehydrogenation reaction on undoped and doped nanostructured carbon catalysts[J]. Chem. Asian. J., 2013, 8: 2605-2608
[37]	Zhou K, Li B, Zhang Q, Huang J Q, Tian G L, Jia J C, Zhao M Q, Luo G H, Su D S, Wei F. The catalytic pathways of hydrohalogenation over metal-free nitrogen-doped carbon nanotubes[J]. ChemSusChem, 2014, 7: 723-728
[38]	Lu X, Chen Z F. Curved Pi-conjugation, aromaticity, and the related chemistry of small fullerenes (Chem. Rev., 2005, 105: 3643-3696
[39]	Hu X, Wu Y, Li H, Zhang Z. Adsorption and activation of O2 on nitrogen-doped carbon nanotubes[J]. J. Phys. Chem. C, 2010, 114: 9603-9607
[40]	Yang Z, Yao Z, Li G, Fang G, Nie H, Liu Z, Zhou X, Chen X, Huang S. Sulfur-doped graphene as an efficient metal-free cathode catalyst for oxygen reduction[J]. ACS Nano, 2012, 6: 205-211
[41]	Montes-Moran M A, Menendez J A, Fuente E, Suarez D. Contribution of the basal planes to carbon basicity: an ab initio study of the H3O+-Pi interaction in cluster models[J]. J. Phys. Chem. B, 1998, 102: 5595-5601
[42]	Suarez D, Menendez J A, Fuente E, Montes-Moran M A. Contribution of pyrone-type structures to carbon basicity: an ab initio study[J]. Langmuir, 1999, 15: 3897-3904
[43]	Menendez J A, Suarez D, Fuente E, Montes-Moran M A. Contribution of pyrone-type structures to carbon basicity: theoretical evaluation of the pK(a) of model compounds[J]. Carbon, 1999, 37: 1002-1006
[44]	Arrigo R, Havecker M, Wrabetz S, Blume R, Lerch M, McGregor J, Parrott E P J, Zeitler J A, Gladden L F, Knop-Gericke A, Schlögl R, Su D S. Tuning the acid/base properties of nanocarbons by functionalization via amination[J]. J. Am. Chem. Soc., 2010, 132: 9616-9630
[45]	Yuan C F, Chen W F, Yan L F. Amino-grafted graphene as a stable and metal-free solid basic catalyst[J]. J. Mater. Chem., 2012, 22: 7456-7460
[46]	Villa A, Tessonnier J P, Majoulet O, Su D S, Schlögl R. Transesterification of triglycerides using nitrogen-functionalized carbon nanotubes[J]. ChemSusChem, 2010, 3: 241-245