ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2015,Vol.31>> Issue(7)>> 1383-1390     doi: 10.3866/PKU.WHXB201504292         中文摘要
Preparation of Manganese Oxides Supported on Graphene Catalysts and Their Activity in Low-Temperature NH3-SCR
JIAO Jin-Zhen1, LI Shi-Hui1, HUANG Bi-Chun1,2
1 College of Environment and Energy, South China University of Technology, Guangzhou 510006, P. R. China;
2 Key Laboratory of the Ministry of Education for Pollution Control and Ecosystem Restoration in Industry Clusters, South China University of Technology, Guangzhou 510006, P. R. China
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Graphene oxide (GO) was synthesized using an improved Hummers method. Subsequently, catalysts of manganese oxides (at varying loadings) supported on graphene (MnOx/GR) were prepared by hydrothermal reaction for application in the selective catalytic reduction (SCR) of NOx with NH3 at low temperatures. The structural properties and catalytic performance were evaluated by Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, X-ray powder diffraction (XRD), transmission electron microscopy (TEM), N2 adsorption-desorption, X-ray photoelectron spectroscopy (XPS), and H2 temperature-programmed reduction (H2-TPR). The characterization results indicated that abundant functional groups existed on the surface of the prepared GO that could combine with manganese during preparation of the catalysts. Manganese oxide entities, with different crystallinities (MnO, Mn3O4, or MnO2), were dispersed on the surface of graphene. The results of the catalytic studies showed that the MnOx/GR catalysts prepared with different MnOx loadings all exhibited excellent low-temperature SCR activities. The catalyst with 20%(w) MnOx displayed the best activity, which was attributed to the high content of high-valent manganese and oxygen adsorbed onto the catalyst surface, as well as to the enhancement in redox abilities and the addition of active sites at low temperatures.

Keywords: Selective catalytic reduction   Nitrogen oxide   Graphene   Graphene oxide   Manganese oxide  
Received: 2015-01-07 Accepted: 2015-04-27 Publication Date (Web): 2015-04-29
Corresponding Authors: HUANG Bi-Chun Email:

Fund: The project was supported by the National Natural Science Foundation of China (51478191).

Cite this article: JIAO Jin-Zhen, LI Shi-Hui, HUANG Bi-Chun. Preparation of Manganese Oxides Supported on Graphene Catalysts and Their Activity in Low-Temperature NH3-SCR[J]. Acta Phys. -Chim. Sin., 2015,31 (7): 1383-1390.    doi: 10.3866/PKU.WHXB201504292

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61. SUN Chao, YAN Liu-Ming, YUE Bao-Hua.Improvement of Surface Structure and Enhancement of Conductivity of LiFePO4 Surface by Graphene and Graphene-Like B-C-N Coating[J]. Acta Phys. -Chim. Sin., 2013,29(08): 1666-1672
62. LI Le, HE Yun-Qiu, CHU Xiao-Fei, LI Yi-Ming, SUN Fang-Fang, HUANG He-Zhou.Hydrothermal Synthesis of Partially Reduced Graphene Oxide-K2Mn4O8 Nanocomposites as Supercapacitors[J]. Acta Phys. -Chim. Sin., 2013,29(08): 1681-1690
63. SHI Qin, MEN Chun-Yan, LI Juan.Preparation and Electrochemical Capacitance Properties of Graphene Oxide/Polypyrrole Intercalation Composite[J]. Acta Phys. -Chim. Sin., 2013,29(08): 1691-1697
64. SHI Lin, YU Tie, WANG Xin-Quan, WANG Jun, SHEN Mei-Qing.Properties and Roles of Adsorbed NH3 and NOx over Cu/SAPO-34 Zeolite Catalyst in NH3-SCR Process[J]. Acta Phys. -Chim. Sin., 2013,29(07): 1550-1557
65. ZHU Qi-Rong, LI Hui-Qin, LI Ning, CHAI Jing, GAO Run-Gang, LIANG Qi.Nanotribological and Wear Properties of Graphene[J]. Acta Phys. -Chim. Sin., 2013,29(07): 1582-1587
66. LONG Mei, CONG Ye, LI Xuan-Ke, CUI Zheng-Wei, DONG Zhi-Jun, YUAN Guan-Ming.Hydrothermal Synthesis and Photocatalytic Activity of Partially Reduced Graphene Oxide/TiO2 Composite[J]. Acta Phys. -Chim. Sin., 2013,29(06): 1344-1350
67. WANG Qiang, HUANG Li-Ping, YU Hong-Tao, QUAN Xie, CHEN Guo-Hua.Recent Developments of Graphene Electrodes in Bioelectrochemical Systems[J]. Acta Phys. -Chim. Sin., 2013,29(05): 889-896
68. XU Jing, ZHU Yong-Fa.Elimination of Bisphenol A from Water via Graphene Oxide Adsorption[J]. Acta Phys. -Chim. Sin., 2013,29(04): 829-836
69. TANG Peng, XIAO Jian-Jian, ZHENG Chao, WANG Shi, CHEN Run-Feng.Graphene-Like Molybdenum Disulfide and Its Application in Optoelectronic Devices[J]. Acta Phys. -Chim. Sin., 2013,29(04): 667-677
70. XU Gui-Yin, DING Bing, NIE Ping, LUO Hong-Jun, ZHANG Xiao-Gang.Preparation and Electrochemical Performance of Carbon Nanotubes/ Graphene Oxide/Sulfur Complex Cathode Material[J]. Acta Phys. -Chim. Sin., 2013,29(03): 546-552
71. GAN Yong-Ping, QIN Huai-Peng, HUANG Hui, TAO Xin-Yong, FANG Jun-Wu, ZHANG Wen-Kui.Preparation and Photocatalytic Activity of Rutile TiO2-Graphene Composites[J]. Acta Phys. -Chim. Sin., 2013,29(02): 403-410
72. ZOU Hui, NI Xiang, PENG Sheng-Lin, OUYANG Jun, CHEN Yu, OUYANG Fang-Ping.First-Principles Study of Graphene-Based Biomolecular Sensor[J]. Acta Phys. -Chim. Sin., 2013,29(02): 250-254
73. HUANG Ping, PAN Si-Wei, HUANG Bi-Chun, CHENG Hua, YE Dai-Qi, WU Jun-Liang, FU Ming-Li, LU Sheng-Liang.Structural Properties of MnOx/Al-SBA-15 in Low-Temperature Selective Catalytic Reduction of NOx with NH3[J]. Acta Phys. -Chim. Sin., 2013,29(01): 176-182
74. WANG Hong-Zhi, GAO Cui-Xia, ZHANG Peng, YAO Su-Wei, ZHANG Wei-Guo.Synthesis and Electrochemical Performance of Graphene/Polyaniline[J]. Acta Phys. -Chim. Sin., 2013,29(01): 117-122
75. WANG Wan-Li, MA Zi-Feng.Synthesis and Characteristics of Pt/graphene by Co-Reduction Method for Oxygen Reduction Reactions[J]. Acta Phys. -Chim. Sin., 2012,28(12): 2879-2884
76. LI Song-Mei, WANG Bo, LIU Jian-Hua, YU Mei, AN Jun-Wei.Synthesis and Microwave Absorption Properties of Nickel Nanoparticles-Graphene Composites with Different Morphologies[J]. Acta Phys. -Chim. Sin., 2012,28(11): 2754-2760
77. SU Peng, GUO Hui-Lin, PENG San, NING Sheng-Ke.Preparation of Nitrogen-Doped Graphene and Its Supercapacitive Properties[J]. Acta Phys. -Chim. Sin., 2012,28(11): 2745-2753
78. LING Xi, ZHANG Jin.Investigation of the Adsorption Behavior of PbPc on Graphene by Raman Spectroscopy[J]. Acta Phys. -Chim. Sin., 2012,28(10): 2355-2362
79. ZHANG Yan-Feng, GAO Teng, ZHANG-Yu, LIU Zhong-Fan.Controlled Growth of Graphene on Metal Substrates and STM Characterizations for Microscopic Morphologies[J]. Acta Phys. -Chim. Sin., 2012,28(10): 2456-2464
80. FAN Cheng-Wei, ZHANG Xin, CHEN Sheng, WANG Hai-Fang, CAO Ao-Neng.Solution-Processable, Highly Conductive, Permanently Rippled Graphene Sheets[J]. Acta Phys. -Chim. Sin., 2012,28(10): 2465-2470
81. LUO Hong-Cheng, HUANG Bi-Chun, FU Ming-Li, WU Jun-Liang, YE Dai-Qi.SO2 Deactivation Mechanism of MnOx/MWCNTs Catalyst for Low-Temperature Selective Catalytic Reduction of NOx by Ammonia[J]. Acta Phys. -Chim. Sin., 2012,28(09): 2175-2182
82. ZHANG Jun-Jun, ZHANG Zhen-Hua, GUO Chao, LI Jie, DENG Xiao-Qing.Electronic Transport Properties for a Zigzag-Edged Triangular Graphene[J]. Acta Phys. -Chim. Sin., 2012,28(07): 1701-1706
83. DAI Yun, LI Jun-Hua, PENG Yue, TANG Xing-Fu.Effects of MnO2 Crystal Structure and Surface Property on the NH3-SCR Reaction at Low Temperature[J]. Acta Phys. -Chim. Sin., 2012,28(07): 1771-1776
84. SHEN Bao-Shou, FENG Wang-Jun, LANG Jun-Wei, WANG Ru-Tao, TAI Zhi-Xin, YAN Xing-Bin.Nitric Acid Modification of Graphene Nanosheets Prepared by Arc- Discharge Method and Their Enhanced Electrochemical Properties[J]. Acta Phys. -Chim. Sin., 2012,28(07): 1726-1732
85. RAN Ke, CHEN Qing, ZUO Jian-Min.Fabrication and Structure Characterization of Quasi-2-Dimensional Amorphous Carbon Structures[J]. Acta Phys. -Chim. Sin., 2012,28(07): 1551-1555
86. ZHANG Xiao, YANG Rong, WANG Chen, HENG Cheng-Lin.Cell Biocompatibility of Functionalized Graphene Oxide[J]. Acta Phys. -Chim. Sin., 2012,28(06): 1520-1524
87. MAAi-Jing, WANG Shao-Zeng, ZOU Hong-Hu, MENG Ming, LI Zhi-Jun, BAO Jun, LI Xin-Gang.The Performance of the NOx Storage Capacity and Sulfur Tolerance of the La0.7Sr0.3Co1-xFexO3 Catalyst[J]. Acta Phys. -Chim. Sin., 2012,28(06): 1474-1480
88. ZHANG Qiu-Lin, XU Hai-Di, QIU Chun-Tian, LIN Tao, GONG Mao-Chu, CHEN Yao-Qiang.Catalytic Performance and Steady-State Kinetics of Cu-ZSM-5 for Selective Catalytic Reduction of NO with NH3[J]. Acta Phys. -Chim. Sin., 2012,28(05): 1230-1236
89. LIU Bo, SUN Hong-Juan, PENG Tong-Jiang.Factor Group Analysis of Molecular Vibrational Modes of Graphene and Density Functional Calculations[J]. Acta Phys. -Chim. Sin., 2012,28(04): 799-804
90. ZHUANG Ke, QIU Jing, XU Bo-Lian, FAN Yi-Ning.Promotional Effect of Cerium Oxide on the Catalytic Properties of Ce-Mn-Ti-O Catalysts for Selective Catalytic Reduction of NO[J]. Acta Phys. -Chim. Sin., 2012,28(03): 681-685
91. JIN Yu, CHEN Hong-Yuan, CHEN Ming-Hai, LIU Ning, LI Qing-Wen.Carbon Nanotube/Polyaniline/Graphene Composite Paper and Its Electrochemical Capacitance Behaviors[J]. Acta Phys. -Chim. Sin., 2012,28(03): 609-614
92. XIE Peng-Yang, ZHUANG Gui-Lin, LÜ Yong-An, WANG Jian-Guo, LI Xiao-Nian.Enhanced Bonding between Noble Metal Adatoms and Graphene with Point Defects[J]. Acta Phys. -Chim. Sin., 2012,28(02): 331-337
93. YANG Xing-Ye, LI Bin, SUN Liang, HUANG Zhi-Wei, CHENG Xiao-Min, ZHANG Tao-Wei, TANG Xing-Fu.Effect of Surface Structure of α-Fe2O3 on the Selective Catalytic Reduction of NO by NH3[J]. Acta Phys. -Chim. Sin., 2012,28(01): 184-188
94. XU Ke, SHEN Lai-Fa, MI Chang-Huan, ZHANG Xiao-Gang.Synthesis and Electrochemical Performance of Graphene Modified LiFePO4 Cathode Materials[J]. Acta Phys. -Chim. Sin., 2012,28(01): 105-110
95. ZHANG Xiao-Yan, SUN Ming-Xuan, SUN Yu-Jun, LI Jing, SONG Peng, SUN Tong, CUI Xiao-Li.Photoelectrochemical Properties of Graphene Oxide Thin Film Electrodes[J]. Acta Phys. -Chim. Sin., 2011,27(12): 2831-2835
96. TANG Jun, KANG Chao-Yang, LI Li-Min, XU Peng-Shou.Direct Graphene Growth by Depositing Carbon Atoms on Si Substrate Covered by SiC Buffer Layers[J]. Acta Phys. -Chim. Sin., 2011,27(12): 2953-2959
97. YANG Xiao-Wei, HE Yu-Shi, LIAO Xiao-Zhen, MA Zi-Feng.Improved Graphene Film by Reducing Restacking for Lithium Ion Battery Applications[J]. Acta Phys. -Chim. Sin., 2011,27(11): 2583-2586
98. LU Xiang-Jun, DOU Hui, YANG Su-Dong, HAO Liang, ZHANG Fang, ZHANG Xiao-Gang.Fabrication and Electrochemical Capacitive Behavior of Freestanding Graphene/Polyaniline Nanofibre Film[J]. Acta Phys. -Chim. Sin., 2011,27(10): 2333-2339
99. YUAN Wen-Hui, LI Bao-Qing, LI Li.Superior Graphene for Hydrogen Adsorption Prepared by the Improved Liquid Oxidation-Reduction Method[J]. Acta Phys. -Chim. Sin., 2011,27(09): 2244-2250
100. MIN Shi-Xiong, Lü Gong-Xuan.Preparation of CdS/Graphene Composites and Photocatalytic Hydrogen Generation from Water under Visible Light Irradiation[J]. Acta Phys. -Chim. Sin., 2011,27(09): 2178-2184
101. YING Hong, WANG Zhi-Yong, GUO Zheng-Duo, SHI Zu-Jin, YANG Shang-Feng.Reduced Graphene Oxide-Modified Bi2WO6 as an Improved Photocatalyst under Visible Light[J]. Acta Phys. -Chim. Sin., 2011,27(06): 1482-1486
102. ZHANG Yi, CHEN Biao, YANG Zu-Pei, ZHANG Zhi-Jun.Controlled Synthesis and Characterization of the Structure and Property of Fe3O4 Nanoparticle-Graphene Oxide Composites[J]. Acta Phys. -Chim. Sin., 2011,27(05): 1261-1266
103. SUN Da-Li, PENG Sheng-Lin, OUYANG Jun, OUYANG Fang-Ping.Electronic Transport Properties of Graphene Nanoribbons with Nanoholes[J]. Acta Phys. -Chim. Sin., 2011,27(05): 1103-1107
104. LI Yun-Xia, WEI Zi-Dong, ZHAO Qiao-Ling, DING Wei, ZHANG Qian, CHEN Si-Guo.Preparation of Pt/Graphene Catalyst and Its Catalytic Performance for Oxygen Reduction[J]. Acta Phys. -Chim. Sin., 2011,27(04): 858-862
105. YANG Yong-Hui, SUN Hong-Juan, PENG Tong-Jiang, HUANG Qiao.Synthesis and Structural Characterization of Graphene-Based Membranes[J]. Acta Phys. -Chim. Sin., 2011,27(03): 736-742
106. DAI Xian-Qi, LI Yan-Hui, ZHAO Jian-Hua, TANG Ya-Nan.Effects of Vacancy and Boron Doping on Si Adsorption on Graphene[J]. Acta Phys. -Chim. Sin., 2011,27(02): 369-373
107. SHEN Bo-Xiong, LIU Ting.Deactivation of MnOx-CeOx/ACF Catalysts for Low-Temperature NH3-SCR in the Presence of SO2[J]. Acta Phys. -Chim. Sin., 2010,26(11): 3009-3016
108. WU Xiao-Qin, ZONG Rui-Long, MU Hao-Jie, ZHU Yong-Fa.Cataluminescence Performance on Catalysts of Graphene Supported Platinum[J]. Acta Phys. -Chim. Sin., 2010,26(11): 3002-3008
109. LIU Jie-Xiang, ZHANG Xiao-Guang, DUAN Zhong-Yu, LIU Xiao-Li.NOx Molecule Adsorption in [Ag]-MAPO-5 (M=Si, Ti)Molecular Sieves[J]. Acta Phys. -Chim. Sin., 2010,26(10): 2679-2685
110. XU Hai-Di, QIU Chun-Tian, ZHANG Qiu-Lin, LIN Tao,GONG Mao-Chu, CHEN Yao-Qiang.Influence of Tungsten Oxide on Selective Catalytic Reduction of NOx with NH3 over MnOx -CeO2 /ZrO2-TiO2Monolith Catalyst[J]. Acta Phys. -Chim. Sin., 2010,26(09): 2449-2454
111. HU Yao-Juan, JIN Juan, ZHANG Hui, WU Ping, CAI Chen-Xin.Graphene: Synthesis, Functionalization and Applications in Chemistry[J]. Acta Phys. -Chim. Sin., 2010,26(08): 2073-2086
112. WEN Zhu-Liang, YANG Su-Dong, SONG Qi-Jun, HAO Liang, ZHANG Xiao-Gang.High Activity of Pd/Graphene Catalysts for Ethanol Electrocatalytic Oxidation[J]. Acta Phys. -Chim. Sin., 2010,26(06): 1570-1574
113. GAN Lin, LIU Song, LI Dan-Na, GU Hang, CAO Yang, SHEN Qian, WANG Zhen-Xing, WANG Qing, GUO Xue-Feng.Facile Fabrication of the Crossed Nanotube-Graphene Junctions[J]. Acta Phys. -Chim. Sin., 2010,26(04): 1151-1156
114. WANG Fan, WANG Yan-Min, WEN Yan-Xuan, SU Hai-Feng, LI Bin.Structural and Morphological Transformation of MnO2 Nanostructures from Mn3O4 Precursor[J]. Acta Phys. -Chim. Sin., 2010,26(02): 521-526
115. TANG Jun, LIU Zhong-Liang, KANG Chao-Yang, YAN Wen-Sheng, XU Peng-Shou, PAN Hai-Bin, WEI Shi-Qiang, GAO Yu-Qiang, XU Xian-Gang.Annealing Time Dependence of Morphology and Structure of Epitaxial Graphene on 6H-SiC(0001) Surface[J]. Acta Phys. -Chim. Sin., 2010,26(01): 253-258
116. CHEN Zhi-Hang, LI Xue-Hui, YANG Qing, LI Hua, GAO Xiang, JIANG Yan-Bin, WANG Fu-Rong, WANG Le-Fu.Removal of NOx Using Novel Fe-Mn Mixed-Oxide Catalysts at Low Temperature[J]. Acta Phys. -Chim. Sin., 2009,25(04): 601-605
117. LIU Jie-Xiang; WEI Xian; ZHANG Xiao-Guang; WANG Gui-Xiang; HAN En-Shan; WANG Jian-Guo.NOx Adsorption in [Ag]-AlMOR Molecular Sieve[J]. Acta Phys. -Chim. Sin., 2009,25(01): 91-96
118. WANG Zhong-Peng; CHEN Ming-Xia; SHANGGUAN Wen-Feng.Simultaneous Catalytic Removal of NOx and Diesel Soot over Cu-Containing Hydrotalcite Derived Catalysts[J]. Acta Phys. -Chim. Sin., 2009,25(01): 79-85
119. YANG Shun-Yi; WANG Xian-You; WEI Jian-Liang; LI Xiu-Qin; TANG An-Ping.Preparation and Electrochemical Performance of Na-Mn-O Cathode Materials[J]. Acta Phys. -Chim. Sin., 2008,24(09): 1669-1674
120. SUN Qi; REN Liang; NIU Jin-Hai; SONG Zhi-Min.Interactions of Dielectric Barrier Discharge Plasmas with NO or NO/O2 Adsorbed on CuZSM-5[J]. Acta Phys. -Chim. Sin., 2008,24(07): 1214-1218
121. LIN Tao; LI Wei; GONG Mao-Chu; YU Yao; DU Bo; CHEN Yao-Qiang.Prepareration of ZrO2-TiO2-CeO2 and Its Application in the Selective Catalytic Reduction of NO with NH3[J]. Acta Phys. -Chim. Sin., 2007,23(12): 1851-1856
122. FANG Hua;CAI Li;LIU Ping;ZHAO Ming;ZHANG Li-Juan;GONG Mao-Chu;CHEN Yao-Qiang .Selective Catalytic Reduction of NO by CH4 on Platinum-Based Monolith Catalysts[J]. Acta Phys. -Chim. Sin., 2006,22(08): 1004-1009
123. XIAO Jian-Hua;LI Xue-Hui;DENG Sha;XU Jian-Chang;WANG Le-Fu.The NOx Oxidation-Storage and Tolerance of SO2 Poison of Mn/Ba/Al2O3 Catalyst[J]. Acta Phys. -Chim. Sin., 2006,22(07): 815-819
124. ZHUANG Quan-chao; FAN Xiao-yong; XU Jin-mei; CHEN Zuo-feng; DONG Quan-feng; JIANG Yan-xia; HUANG Ling; SUN Shi-gang.Electrochemical Impedance Spectroscopic Study of the First Delithiation of Spinel Lithium Manganese Oxide[J]. Acta Phys. -Chim. Sin., 2006,22(02): 234-238
125. PEI Mei-Xiang; LIN He; SHANGGUAN Wen-Feng; HUANG Zhen.The Effects of Plasma on Simultaneously Catalytic Removal of NOx and Soot[J]. Acta Phys. -Chim. Sin., 2005,21(03): 255-260
126. KANG Shou-Fang; JIANG Zheng; HAO Zheng-Ping.Influence of Cu on NOx Storage Performance of Pt/Cu-Mg-Al-O Catalysts Derived from Hydrotalcites[J]. Acta Phys. -Chim. Sin., 2005,21(03): 278-282
127. SUN Qi;ZHU Ai-Min;NIU Jin-Hai;XU Yong;SONG Zhi-Min.Plasma-induced Conversion of Nitrogen Oxides in a Dielectric Barrier Discharge Reactor[J]. Acta Phys. -Chim. Sin., 2005,21(02): 192-196
128. Zhao Li-Li;Wang Rong-Shu.Preparation of MnO2(Li) and Its Ion Exchange Kinetics[J]. Acta Phys. -Chim. Sin., 2003,19(10): 933-937
129. WANG Cheng-Xian, YU Fei, MA Jie.Applications of Graphene-based Hybrid Material as Electrodes in Microbial Fuel Cells[J]. Acta Phys. -Chim. Sin., 0,(): 0-0
130. ZHU Jie-Jun, SUN Hai-Bin, WU Yao-Zheng, WAN Jian-Guo, WANG Guang-Hou.Graphene: Synthesis, Characterization and Application in Transparent Conductive Films[J]. Acta Phys. -Chim. Sin., 0,(): 0-0
131. WANG Yun-Jing, LIU Ying-Qiu, GAO Xiu-Xiu, ZHAN Yan-Shan, PAN Li-Yang, ZHANG Wen-Kai, FANG Xiao-Min.Surface Defects Passivation of Graphene Quantum Dots by Amino Functionalization and its Photoluminescence Emission Enhancement[J]. Acta Phys. -Chim. Sin., 0,(): 0-0
132. LIANG Jia-Xu, XIAO Zhi-Chang, ZHI Lin-Jie.Graphenal Polymers: 3D Carbon-rich Polymers as Energy Materials with both Electronic and Ionic Transport Path[J]. Acta Phys. -Chim. Sin., 0,(): 0-0
133. XIA Kai-Lun, JIAN Mu-Qiang, ZHANG Ying-Ying.Advances in Flexible Conductors Based on Nanocarbon Materials[J]. Acta Phys. -Chim. Sin., 0,(): 0-0
134. LI Guang-Yong, WU Xiao-Han, HE Wei-Na, FANG Jian-Hui, ZHANG Xue-Tong.Controlled Assembly of the Graphene-based Aerogel[J]. Acta Phys. -Chim. Sin., 0,(): 0-0
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