
北京建筑大学机电与车辆工程学院,北京市 西城区 100044
[ "王海光(1980),男,博士研究生,研究方向为氢能与燃料电池技术,richgas@126.com;" ]
[ "刘永峰(1973),男,博士,教授,研究方向为氢能与车辆燃料电池技术,本文通信作者,liuyongfeng@bucea.edu.cn;" ]
[ "张军(1972),男,博士,教授,研究方向为车辆/轨道系统动力学,zhangjun611@bucea.edu.cn。" ]
收稿日期:2022-12-01,
纸质出版日期:2023-06-30
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王海光,刘永峰,张军.氮掺杂介孔碳负载钴催化剂的制备及其脱除富氢气体CO性能研究[J].发电技术,2023,44(03):373-381.
WANG Haiguang,LIU Yongfeng,ZHANG Jun.Preparation of Nitrogen Doped Mesoporous Carbon Supported Cobalt Catalyst and Its Performance for Removal of CO in Hydrogen-Rich Gas[J].Power Generation Technology,2023,44(03):373-381.
王海光,刘永峰,张军.氮掺杂介孔碳负载钴催化剂的制备及其脱除富氢气体CO性能研究[J].发电技术,2023,44(03):373-381. DOI: 10.12096/j.2096-4528.pgt.22142.
WANG Haiguang,LIU Yongfeng,ZHANG Jun.Preparation of Nitrogen Doped Mesoporous Carbon Supported Cobalt Catalyst and Its Performance for Removal of CO in Hydrogen-Rich Gas[J].Power Generation Technology,2023,44(03):373-381. DOI: 10.12096/j.2096-4528.pgt.22142.
为有效脱除富氢气体中的CO,制备了氮掺杂的有序介孔碳及其负载纳米钴颗粒的催化剂,采用N
2
吸附-脱附、X射线衍射(X-ray diffraction,XRD)、拉曼光谱、X射线光电子能谱(X-ray photoelectron spectroscopy,XPS)、热重-质谱联用(thermogravimetry-mass spectrometry,TG-MS)等手段进行表征,研究了氮掺杂对有序介孔碳负载钴基催化剂的自还原行为和CO甲烷化反应性能的影响规律。结果表明,在介孔碳骨架中引入的氮原子主要作为氧化钴的成核位点,与氧化物载体产生较强的相互作用,大大提高了钴物种的分散度,从而形成颗粒尺寸均匀的小纳米钴颗粒,显著促进了其自还原反应,进而提高了催化剂的还原度。催化剂评价结果表明,与未掺杂氮的介孔碳载体相比,氮掺杂介孔碳载体使催化剂的CO脱除效率明显提升。
In order to effectively remove CO from hydrogen-rich gas
cobalt-based nano-particle catalyst supported on nitrogen-doped ordered mesoporous carbon was prepared and characterized by X-ray diffraction (XRD)
Raman spectrum
X-ray photoelectron spectroscopy (XPS) and thermogravimetry-mass spectrometry (TG-MS). The effects of nitrogen doping on the self-reduction behavior of the catalyst and CO methanation reaction performance were studied. The characterization results show that the nitrogen atoms introduced into the mesoporous carbon skeleton are mainly used as the nucleation sites of cobalt oxide
which have a strong interaction with the oxide carrier
and greatly improve the dispersion of cobalt species. Thus
small nano-cobalt particles with uniform particle size are formed
which significantly promote self-reduction reaction and thereby improve the reduction degree of the catalyst. The catalyst evaluation results show that
compared with the mesoporous carbon carrier without doping
the CO removal efficiency of the catalyst doped by nitrogen is much higher.
杨馥源 , 田雪沁 , 徐彤 , 等 . 面向碳中和电力系统转型的电氢枢纽灵活性应用 [J ] . 电力建设 , 2021 , 42 ( 8 ): 110 - 117 . doi: 10.12204/j.issn.1000-7229.2021.08.013 http://dx.doi.org/10.12204/j.issn.1000-7229.2021.08.013
YANG F Y , TIAN X Q , XU T , et al . Flexibility of electro-hydrogen hub for power system transformation under the goal of carbon neutrality [J ] . Electric Power Construction , 2021 , 42 ( 8 ): 110 - 117 . doi: 10.12204/j.issn.1000-7229.2021.08.013 http://dx.doi.org/10.12204/j.issn.1000-7229.2021.08.013
曹蕃 , 郭婷婷 , 殷爱鸣 , 等 . 风光氢混合发电系统设计与能量管理策略研究进展 [J ] . 分布式能源 , 2021 , 26 ( 4 ): 1 - 14 .
CAO F , GUO T T , YIN A M , et al . Research progress on optimal sizing and energy management strategy of wind-solar-hydrogen hybrid energy systems [J ] . Distributed Energy , 2021 , 26 ( 4 ): 1 - 14 .
黄倬 , 屠海令 , 张冀强 , 等 . 质子交换膜燃料电池的开发与应用 [M ] . 北京 : 冶金工业出版社 , 2000 : 5 - 29 .
HUANG Z , TU H L , ZHANG J Q , et al . Development and application of proton exchange membrane fuel cells [M ] . Beijing : Metallurgical Industry Press , 2000 : 5 - 29 .
黄莎华 , 刘之景 , 王支逸 . 燃料电池开发现状及其发展趋势 [J ] . 化学通报 , 2004 , 67 ( 7 ): 551 - 557 . doi: 10.3969/j.issn.0441-3776.2004.07.006 http://dx.doi.org/10.3969/j.issn.0441-3776.2004.07.006
HUANG S H , LIU Z J , WANG Z Y . Survey of the present condition of fuel cell and its development tendency [J ] . Chemistry , 2004 , 67 ( 7 ): 551 - 557 . doi: 10.3969/j.issn.0441-3776.2004.07.006 http://dx.doi.org/10.3969/j.issn.0441-3776.2004.07.006
赵海贺 , 陈泽宇 , 覃承富 , 等 . 车用燃料电池氢气循环系统引射特性研究 [J ] . 电力工程技术 , 2022 , 41 ( 1 ): 173 - 179 . doi: 10.12158/j.2096-3203.2022.01.023 http://dx.doi.org/10.12158/j.2096-3203.2022.01.023
ZHAO H H , CHEN Z Y , QIN C F , et al . Ejection characteristics of hydrogen cycle system for vehicular fuel cell [J ] . Electric Power Engineering Technology , 2022 , 41 ( 1 ): 173 - 179 . doi: 10.12158/j.2096-3203.2022.01.023 http://dx.doi.org/10.12158/j.2096-3203.2022.01.023
李林 , 刘彤宇 , 李爽 , 等 . 甲醇重整制氢燃料电池发电研究进展 [J ] . 发电技术 , 2022 , 43 ( 1 ): 44 - 53 . doi: 10.12096/j.2096-4528.pgt.21116 http://dx.doi.org/10.12096/j.2096-4528.pgt.21116
LI L , LIU T Y , LI S , et al . Research progress of hydrogen production by methanol reforming for fuel cell power generation [J ] . Power Generation Technology , 2022 , 43 ( 1 ): 44 - 53 . doi: 10.12096/j.2096-4528.pgt.21116 http://dx.doi.org/10.12096/j.2096-4528.pgt.21116
陈清泉 , 孙立清 . 电动汽车的现状和发展趋势 [J ] . 科技导报 , 2005 , 23 ( 4 ): 24 - 28 . doi: 10.3321/j.issn:1000-7857.2005.04.008 http://dx.doi.org/10.3321/j.issn:1000-7857.2005.04.008
CHEN Q Q , SUN L Q . Present status and future trends of electric vehicles [J ] . Science and Technology Review , 2005 , 23 ( 4 ): 24 - 28 . doi: 10.3321/j.issn:1000-7857.2005.04.008 http://dx.doi.org/10.3321/j.issn:1000-7857.2005.04.008
王海光 , 刘永峰 , 张军 . 富氢气体脱除CO催化剂的制备及性能研究 [J ] . 发电技术 , 2022 , 43 ( 6 ): 901 - 907 . doi: 10.12096/j.2096-4528.pgt.22014 http://dx.doi.org/10.12096/j.2096-4528.pgt.22014
WANG H G , LIU Y F , ZHANG J . Preparation and its performance of catalyst for CO removal from hydrogen rich gas mixture [J ] . Power Generation Technology , 2022 , 43 ( 6 ): 901 - 907 . doi: 10.12096/j.2096-4528.pgt.22014 http://dx.doi.org/10.12096/j.2096-4528.pgt.22014
SONG S Q , TSIAKARAS P . Recent progress indirect ethanol proton exchange membrane fuel cells (DE-PEMFC) [J ] . Applied Catalysis B:Environmental , 2006 , 63 ( 3/4 ): 187 - 193 . doi: 10.1016/j.apcatb.2005.09.018 http://dx.doi.org/10.1016/j.apcatb.2005.09.018
刘其海 . 富氢重整气中CO选择性甲烷化剂催化剂的研究 [D ] . 广州 : 华南理工大学 , 2009 .
LIU Q H . Study on selective CO mathanation catalysts in hydrogen-rich gases [D ] . Guangzhou : South China University of Technology , 2009 .
严菁 , 马建新 , 万钢 . 用于燃料电池汽车重整器的CO脱除技术 [J ] . 天然气化工 , 2002 , 27 ( 5 ): 35 - 38 . doi: 10.3969/j.issn.1001-9219.2002.05.010 http://dx.doi.org/10.3969/j.issn.1001-9219.2002.05.010
YAN J , MA J X , WAN G . Methods of CO clean-up for the reformer of fuel cell vehicles [J ] . Natural Gas Chemical Industry , 2002 , 27 ( 5 ): 35 - 38 . doi: 10.3969/j.issn.1001-9219.2002.05.010 http://dx.doi.org/10.3969/j.issn.1001-9219.2002.05.010
纪玉国 , 赵震 , 余长春 , 等 . Fischer-Tropsch合成钴基催化剂研究进展 [J ] . 化工进展 , 2007 , 26 ( 7 ): 927 - 933 . doi: 10.3321/j.issn:1000-6613.2007.07.004 http://dx.doi.org/10.3321/j.issn:1000-6613.2007.07.004
JI Y G , ZHAO Z , YU C C , et al . Progress of cobalt-based catalysts in Fischer-Tropsch synthesis [J ] . Chemical Industry and Engineering Progress , 2007 , 26 ( 7 ): 927 - 933 . doi: 10.3321/j.issn:1000-6613.2007.07.004 http://dx.doi.org/10.3321/j.issn:1000-6613.2007.07.004
IGLESIA E , SOLED S L , FIANTO R A . Fischer-Tropsch synthesis on cobalt and ruthenium metal dispersion and support effects on reaction and selectivity [J ] . Journal of Catalysis , 1992 , 137 ( 1 ): 212 - 224 . doi: 10.1016/0021-9517(92)90150-g http://dx.doi.org/10.1016/0021-9517(92)90150-g
李晨 , 马向东 , 应为勇 , 等 . Co-Ru/γ-Al 2 O 3 催化剂的F-T合成性能 [J ] . 石油化工 , 2008 , 37 ( 1 ): 34 - 38 . doi: 10.3321/j.issn:1000-8144.2008.01.007 http://dx.doi.org/10.3321/j.issn:1000-8144.2008.01.007
LI C , MA X D , YING W Y , et al . Catalytic performance of Co-Ru/γ-Al 2 O 3 catalyst for Ficher-Tropsch synthesis [J ] . Petrochemical Technology , 2008 , 37 ( 1 ): 34 - 38 . doi: 10.3321/j.issn:1000-8144.2008.01.007 http://dx.doi.org/10.3321/j.issn:1000-8144.2008.01.007
李剑锋 , 侯学锋 , 代小平 , 等 . 不同载体和前驱体对钴基催化剂浆相费托合成性能的影响 [J ] . 石油大学学报(自然科学版) , 2004 , 28 ( 5 ): 94 - 98 .
LI J F , HOU X F , DAI X P , et al . Effect of supports and precursors on Co-based fine particle catalyst for slurry phase Fischer-Tropsch synthesis [J ] . Journal of China University of Petroleum (Natural Science Edition) , 2004 , 28 ( 5 ): 94 - 98 .
HA K S , KWAK G , JUN K W , et al . Ordered mesoporous carbon nanochannel reactors for high-performance Fischer-Tropsch synthesis [J ] . Chemical Communications , 2013 , 49 ( 45 ): 5141 - 5143 . doi: 10.1039/c3cc00297g http://dx.doi.org/10.1039/c3cc00297g
FU T , JIANG Y , LV J , et al . Effect of carbon support on Fischer-Tropsch synthesis activity and product distribution over Co-based catalysts [J ] . Fuel Processing Technology , 2013 , 110 : 141 - 149 . doi: 10.1016/j.fuproc.2012.12.006 http://dx.doi.org/10.1016/j.fuproc.2012.12.006
RADKEVICH V Z , SENKO T L , WILSON K , et al . The influence of surface functionalization of activated carbon on palladium dispersion and catalytic activity in hydrogen oxidation [J ] . Applied Catalysis A:Genetal , 2008 , 335 ( 2 ): 241 - 251 . doi: 10.1016/j.apcata.2007.11.029 http://dx.doi.org/10.1016/j.apcata.2007.11.029
DEIFALLAH M , MCMILLAN P F , CORA F . Electronic and structural properties of two-dimensional carbon nitride graphenes [J ] . The Journal of Physical Chemistry C , 2008 , 112 ( 14 ): 5447 - 5453 . doi: 10.1021/jp711483t http://dx.doi.org/10.1021/jp711483t
LI X , WANG H , ROBINSON J T , et al . Simultaneous nitrogen doping and reduction of graphene oxide [J ] . Journal of the American Chemical Society , 2009 , 131 ( 43 ): 15939 - 15944 . doi: 10.1021/ja907098f http://dx.doi.org/10.1021/ja907098f
CHEN W , PAN X , WILLINGER M G , et al . Facile autoreduction of iron oxide/carbon nanotube encapsulates [J ] . Journal of the American Chemical Society , 2006 , 128 ( 10 ): 3136 - 3137 . doi: 10.1021/ja056721l http://dx.doi.org/10.1021/ja056721l
CHEN W , PAN X , BAO X . Turing of redox properties of iron and iron oxides via encapsulation within carbon nanotubes [J ] . Journal of the American Chemical Society , 2007 , 129 ( 23 ): 7421 - 7426 . doi: 10.1021/ja0713072 http://dx.doi.org/10.1021/ja0713072
LU A H , LI W C , SCHMIDT W , et al . Easy synthesis of an ordered mosoporous carbon with a hexagonally packed tubular structure [J ] . Carbon , 2004 , 42 ( 14 ): 2939 - 2948 . doi: 10.1016/j.carbon.2004.07.006 http://dx.doi.org/10.1016/j.carbon.2004.07.006
JUN Y S , HONG W H , ANTONIETTI M , et al . 2D hexagonal carbon nitride and titanium nitride/carbon composites [J ] . Advanced Materials , 2009 , 21 ( 42 ): 4270 - 4274 . doi: 10.1002/adma.200803500 http://dx.doi.org/10.1002/adma.200803500
ZHAO Y , LIU Z , CHU W , et al . Large scale synthesis of nitrogen-rich carbon nitride microfibers by using graphitic carbon nitride as precursor [J ] . Advanced Materials , 2008 , 20 ( 9 ): 1777 - 1781 . doi: 10.1002/adma.200702230 http://dx.doi.org/10.1002/adma.200702230
YAN S C , LI Z S , ZOU Z G . Photodegradation performance of g-C 3 N 4 fabricated by directly heating melamine [J ] . Langmuir , 2009 , 25 ( 17 ): 10397 - 10401 . doi: 10.1021/la900923z http://dx.doi.org/10.1021/la900923z
XU X , LI Y , GONG Y , et al . Synthesis of palladium nanopaticles supported on mesoporous N-doped carbon and their catalytic ability for biofuel upgrade [J ] . Journal of the American Chemical Society , 2012 , 134 ( 41 ): 16987 - 16990 . doi: 10.1021/ja308139s http://dx.doi.org/10.1021/ja308139s
ZHAO D , HUO Q , FENG J , et al . Nonionic triblock and star diblock copolymer and oligomeric surfactant syntheses of highly ordered,hydrothermally stable, mesoporous silica structure [J ] . Journal of the American Chemical Society , 1998 , 120 ( 24 ): 6024 - 6036 . doi: 10.1021/ja974025i http://dx.doi.org/10.1021/ja974025i
POON S W , PAN J S , TOK E S . Nucleation and growth of cobalt nanostructures on highly oriented pyrolytic graphite [J ] . Physical Chemistry Chemical Physics , 2006 , 8 ( 28 ): 3326 - 3334 . doi: 10.1039/b604627b http://dx.doi.org/10.1039/b604627b
BEZEMER G L , BITTER J H , KUIPERS H P C E , et al . Cobalt particle size effects in the Fischer-Tropsch reaction studied with carbon nanofiber supported catalysts [J ] . Journal of the American Chemical Society , 2006 , 128 ( 12 ): 3956 - 3964 . doi: 10.1021/ja058282w http://dx.doi.org/10.1021/ja058282w
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