西安交通大学能源与动力工程学院,西安,710049
: 2024-03-25。作者简介: 赵君安(2000—),男,硕士生
王树众(通信作者),男,教授,博士生导师。基金项目: 国家自然科学基金资助项目(52101096
网络首发:2024-11-10,
纸质出版:2024
移动端阅览
赵君安, 刘璐, 王树众, 等. 超临界水热合成纳米氧化锌的动力学及聚乙烯吡咯烷酮耦合作用机理研究[J]. 西安交通大学学报, 2024,58(11):156-163.
ZHAO Jun'an, LIU Lu, WANG Shuzhong, et al. Research on Kinetics and PVP Coupling Mechanism of Nanoscale Zinc Oxide Synthesized by Supercritical Water Hydrothermal Method[J]. 2024, 58(11): 156-163.
赵君安, 刘璐, 王树众, 等. 超临界水热合成纳米氧化锌的动力学及聚乙烯吡咯烷酮耦合作用机理研究[J]. 西安交通大学学报, 2024,58(11):156-163. DOI: 10.7652/xjtuxb202411015.
ZHAO Jun'an, LIU Lu, WANG Shuzhong, et al. Research on Kinetics and PVP Coupling Mechanism of Nanoscale Zinc Oxide Synthesized by Supercritical Water Hydrothermal Method[J]. 2024, 58(11): 156-163. DOI: 10.7652/xjtuxb202411015.
为了获得超临界水热合成过程中纳米氧化锌的结晶动力学机理及表面改性作用机理
分析了温度、时间驱动下的结晶动力学曲线
获得了纳米氧化锌在成核、生长过程的速率及活化能。同时采用聚乙烯吡咯烷酮(PVP)对氧化锌进行原位表面改性
通过分析不同比例PVP和KOH作用下合成的氧化锌形貌
获得了PVP和KOH的耦合作用机理。实验结果表明:纳米氧化锌在成核过程中的活化能为603.06 kJ·mol
-1
在生长过程中的活化能为63.10 kJ·mol
-1
在成核阶段比生长阶段消耗的能量更多; 在前驱物、KOH、PVP的物质的量浓度比为1:3:2 时合成了粒径最小的纳米氧化锌颗粒
平均粒径为6.9 nm; 当KOH、PVP的浓度比过高时
纳米氧化锌颗粒表面过量的PVP使其成为凝胶类沉积物
形成一种团聚体从而导致合成纳米颗粒的粒径变大。
Supercritical hydrothermal synthesis(SCHS)is an efficient and green technology for preparing advanced nano-powders
which can promote the development of high-quality nanoscale ZnO. In order to obtain the crystallization kinetics and surface modification mechanism of nanoscale ZnO during the SCHS process
this paper analyzes the crystallization kinetics curves driven by temperature and time to obtain information on the rates and activation energies of nanoscale ZnO in nucleation and growth processes. Additionally
polyvinylpyrrolidone(PVP)is used to modi
fy ZnO surface in situ. By analyzing the morphology of zinc oxide synthesized under different PVP and KOH ratios
the coupling mechanism of PVP and KOH is determined. The results indicate that the activation energy of nanoscale is 603.06 kJ·mol
-1
during nucleation and 63.10 kJ·mol
-1
during growth
with more energy consumed in the nucleation stage than in the growth stage. Nanoscale ZnO particles with the smallest size are synthesized when the precursor
KOH
and PVP concentration ratio is 1:3:2
with an average particle size of 6.9 nm. When the KOH to PVP concentration ratio is too high
excess PVP on the surface of ZnO nanoparticles leads to gel-like deposits
forming aggregates that result in an increase in the particle size of the synthesized nanoparticles.
ZHANG Hui, YANG Deren, JI Yujie, et al. Low temperature synthesis of flowerlike ZnO nanostructures by cetyltrimethylammonium bromide-assisted hydrothermal process [J]. The Journal of Physical Chemistry: B, 2004, 108(13): 3955-3958.
DEMOISSON F, PIOLET R, BERNARD F. Hydrothermal growth of ZnO nanostructures in supercritical domain: Effect of the metal salt concentration(Zn(NO3)2)in alkali medium(KOH)[J]. The Journal of Supercritical Fluids, 2015, 97: 268-274.
WOJNAROWICZ J, CHUDOBA T, LOJKOWSKI W. A review of microwave synthesis of zinc oxide nanomaterials: reactants, process parameters and morphologies [J]. Nanomaterials, 2020, 10(6): 1086.
DEMOISSON F, PIOLET R, ARIANE M, et al. Influence of the pH on the ZnO nanoparticle growth in supercritical water: experimental and simulation approaches [J]. The Journal of Supercritical Fluids, 2014, 95: 75-83.
HAN N S, SHIM H S, SEO J H, et al. Optical properties and lasing of ZnO nanoparticles synthesized continuously in supercritical fluids [J]. Chemical Physics Letters, 2011, 505(1/2/3): 51-56.
EMANETOGLU N W, GORLA C, LIU Y, et al. Epitaxial ZnO piezoelectric thin films for saw filters [J]. Materials Science in Semiconductor Processing, 1999, 2(3): 247-252.
LIANG S, SHENG H, LIU Y, et al. ZnO schottky ultraviolet photodetectors [J]. Journal of Crystal Growth, 2001, 225(2/4): 110-113.
MITRA P, CHATTERJEE A P, MAITI H S. ZnO thin film sensor [J]. Materials Letters, 1998, 35(1/2): 33-38.
OHARA S, MOUSAVAND T, UMETSU M, et al. Hydrothermal synthesis of fine zinc oxide particles under supercritical conditions [J]. Solid State Ionics, 2004, 172(1/4): 261-264.
汤皎宁, 龚晓钟, 李均钦. 均匀沉淀法制备纳米氧化锌的研究 [J]. 无机材料学报, 2006, 21(1): 65-69.
TANG Jiaoning, GONG Xiaozhong, LI Junqin. Synthesis of nanometer ZnO particles by directly precipitation method [J].Journal of Inorganic Materials, 2006, 21(1): 65-69.
苏照伟, 方莹, 李镇, 等. 水热法制备纳米氧化锌的因素探究 [J]. 中国陶瓷, 2013, 49(6): 13-15.
SU Zhaowei, FANG Ying, LI Zhen, et al. Research on the factors of ZnO nanoparticles prepared by hydrothermal method [J]. China Ceramics, 2013, 49(6): 13-15.
谢云龙, 钟国, 杜高辉. 硫化锌与硫化锌/氧化锌异质结纳米线的化学气相沉积法制备与表征 [J]. 化学学报, 2012, 70(10): 1221-1226.
XIE Yunlong, ZHONG Guo, DU Gaohui. Preparation and characterization of ZnS and ZnS/ZnO heterostructure nanowire by chemical vapor deposition [J]. Acta Chimica Sinica, 2012, 70(10): 1221-1226.
RUIZ-JORGE F, PORTELA J R, SÁNCHEZ-ONETO J, et al. Synthesis of micro-and nanoparticles in sub-and supercritical water: from the laboratory to larger scales [J]. Applied Sciences, 2020, 10(16): 5508.
GOODALL J B M, ILLSLEY D, LINES R, et al. Structure-property-composition relationships in doped zinc oxides: enhanced photocatalytic activity with rare earth dopants [J]. ACS Combinatorial Science, 2015, 17(2): 100-112.
DEMOISSON F, PIOLET R, BERNARD F. Hydrothermal synthesis of ZnO crystals from Zn(OH)2 metastable phases at room to supercritical conditions [J]. Crystal Growth Design, 2014, 14(11): 5388-5396.
毛志强. 超临界(亚临界水)法连续制备形貌可控的纳米氧化锌及其光催化性能 [D]. 上海: 上海交通大学, 2013: 31-32.
SUE K, MURATA K, KIMURA K, et al. Continuous synthesis of zinc oxide nanoparticles in supercritical water [J]. Green Chemistry, 2003, 5(5): 659-662.
SUE K, KIMURA K, ARAI K. Hydrothermal synthesis of ZnO nanocrystals using microreactor [J]. Materials Letters, 2004, 58(25): 3229-3231.
SUE K, KIMURA K, YAMAMOTO M, et al. Rapid hydrothermal synthesis of ZnO nanorods without organics [J]. Materials Letters, 2004, 58(26): 3350-3352.
AKSOMAITYTE G, POLIAKOFF M, LESTER E. The production and formulation of silver nanoparticles using continuous hydrothermal synthesis [J]. Chemical Engineering Science, 2013, 85: 2-10.
KUBOTA S, MORIOKA T, TAKESUE M, et al. Continuous supercritical hydrothermal synthesis of dispersible zero-valent copper nanoparticles for ink applications in printed electronics [J]. The Journal of Supercritical Fluids, 2014, 86: 33-40.
HASSANZADEH N, SADRNEZHAAD S K, GHORBANZADEH M. An investigation of crystallization kinetics of the Na3MnCO3PO4 cathode material, synthesized by the hydrothermal method [J]. Materials Chemistry and Physics, 2018, 214: 73-79.[23] PAN Feng, LU Xuchen, WANG Yun, et al. Synthesis and crystallization kinetics of ZSM-5 without organic template from coal-series kaolinite [J]. Microporous and Mesoporous Materials, 2014, 184: 134-140.
LEITNER J, SEDMIDUBSKY' D, JANKOVSKY' O. Effect of ZnO nanosizing on its solubility in aqueous media [J]. Micro Nano Letters, 2018, 13(11): 1585-1589.
CHERGUI Y, AOUAROUN T, HADLEY M J, et al. Molecular dynamics simulation of ZnO wurtzite phase under high and low pressures and temperatures [J]. Materials Research Express, 2017, 4(11): 115016.
BÉNÉZETH P, PALMER D A, WESOLOWSKI D J, et al. New measurements of the solubility of zinc oxide from 150 to 350 ℃ [J]. Journal of Solution Chemistry, 2002, 31(12): 947-973.
AKINFIEV N N, PLYASUNOV A V. Steam solubilities of solid MoO3, ZnO and Cu2O, calculated on a basis of a thermodynamic model [J]. Fluid Phase Equilibria, 2013, 338: 232-244.
ORITA Y, AKIZUKI M, OSHIMA Y. Kinetic analysis of zinc oxide anisotropic growth in supercritical water [J]. The Journal of Supercritical Fluids, 2019, 154: 104609.
0
浏览量
26
下载量
0
CSCD
关联资源
相关文章
相关作者
相关机构
京公网安备11010802024621