一步醇热法制备纳米CeO2-ZrO2固溶体及其除砷性能

doi:10.15541/jim20250011

无机材料学报

• 研究论文 • 上一篇

一步醇热法制备纳米CeO₂-ZrO₂固溶体及其除砷性能

李荣辉, 钱骏

河北地质大学宝石与材料学院, 河北省岩石矿物材料绿色开发重点实验室, 石家庄 050031

收稿日期:2025-01-08 修回日期:2025-03-05
作者简介:李荣辉(1983-), 男, 讲师. E-mail: lrh031776@163.com
基金资助:
河北地质大学博士科研启动金（BQ2024054）; 石家庄市科技计划（No.2412404301）; 河北省高等教育规划研究课题（2403146）

One-step Alcohothermal Synthesis of Nanocrystalline CeO₂-ZrO₂ Solid Solution and Its Arsenic Removal Performance

LI Ronghui, QIAN Jun

Hebei Key Laboratory of Green Development of Rock Mineral Materials, School of Gemology and Materials Science, Hebei GEO University, Shijiazhuang 050031, China

Received:2025-01-08 Revised:2025-03-05
About author:LI Ronghui (1983-), male, lecture. E-mail: lrh031776@163.com
Supported by:
Ph.D Pesearch Start-up Foundation of Hebei GEO University (BQ2024054); Shijiazhuang Science and Technology Plan (No.2412404301); Higher Education Plan and Research Project of Hebei Province (2403146)

摘要/Abstract

摘要： CeO₂-ZrO₂固溶体的制备一般通过化学沉淀和高温焙烧两步完成,但是在高温条件下,纳米晶粒容易聚集长大,导致其比表面积降低,进而削弱了其吸附和催化性能。本研究通过简单的一步醇热法制备出高比表面积的纳米CeO₂-ZrO₂固溶体,避免了高温焙烧对晶粒长大和比表面积降低的影响。采用不同手段对制备的CeO₂-ZrO₂固溶体的晶体结构、微观形貌以及热稳定性进行表征,测试其除砷性能。结果表明,本方法制备的纳米CeO₂-ZrO₂固溶体的晶粒发育完整,粒子纯度高、分散性好,对水中As(III)具有良好的吸附效果。其中,Ce_0.8Zr_0.2O₂样品在As(III)平衡溶度为95 mg/L时的饱和吸附量可达163 mg/g,高于纯CeO₂和ZrO₂样品,也远高于传统焙烧法制备的CeO₂-ZrO₂固溶体,并且该吸附材料在pH为3~9范围内一直保持较高的As(III)去除率以及良好的耐酸碱性能。吸附机理研究表明,溶液中As(III)离子与Ce_0.8Zr_0.2O₂固溶体表面金属离子形成配位键,该过程属于化学吸附。

关键词: 醇热法, CeO₂-ZrO₂固溶体, 除砷性能, 吸附机理

Abstract: CeO₂-ZrO₂ solid solution is generally synthesized through chemical precipitation, followed by high-temperature calcination. The grains of solid solution under high-temperature calcination are prone to aggregate and grow, resulting in lower specific surface area and weaker adsorption and catalytic performance. In this study, nanocrystalline CeO₂-ZrO₂ solid solutions were prepared by a simple one-step alcohothermal method, avoiding effects of high-temperature calcination on grain growth and specific surface area reduction. The crystal structure, morphologies and thermal stability of the synthesized CeO₂-ZrO₂ solid solution were characterized by different techniques, and arsenic removal performance was tested. The results show that nanocrystalline CeO₂-ZrO₂ solid solutions have complete grain growth with large specific surface areas, high particle purity and good dispersibility, improving adsorption effect on As (III) in water. The arsenic adsorption results show that maximum adsorption capacity of Ce_0.8Zr_0.2O₂ sample can reach 160 mg/g at a As(III) equilibrium solubility of 100 mg/L, which is much higher than pure CeO₂ and ZrO₂ samples, as well as CeO₂-ZrO₂ solid solution prepared by traditional calcination method. In addition, the prepared Ce_0.8Zr_0.2O₂ solid solution maintains a high As (III) removal rate and good acid-alkali resistance within pH range of 3-9. The arsenic adsorption mechanisms indicate that As (III) ions in the solution form coordination bonds with metal ions on the surface of Ce_0.8Zr_0.2O₂solid solution, which belongs to the chemical adsorption process.

Key words: alcohothemal, CeO₂-ZrO₂ solid solution, arsenic removal performance, adsorption mechanism

中图分类号:

O611

李荣辉, 钱骏. 一步醇热法制备纳米CeO₂-ZrO₂固溶体及其除砷性能[J]. 无机材料学报, DOI: 10.15541/jim20250011.

LI Ronghui, QIAN Jun. One-step Alcohothermal Synthesis of Nanocrystalline CeO₂-ZrO₂ Solid Solution and Its Arsenic Removal Performance[J]. Journal of Inorganic Materials, DOI: 10.15541/jim20250011.

参考文献

[1] LI Z J, YANG Q C, YANG Y,et al. Hydrogeochemical controls on arsenic contamination potential and health threat in an intensive agricultural area, northern China. Environmental Pollution, 2020, 256: 113455.
[2] ALIJANI H, SHARIATINIA Z.Effective aqueous arsenic removal using zero valent iron doped MWCNT synthesized byin situ CVD method using natural α-Fe₂O₃ as a precursor. Chemosphere, 2017, 171: 502.
[3] LATA S, SAMADDER S R.Removal of arsenic from water using nano adsorbents and challenges: a review.Journal of Environmental Management, 2016, 166: 387.
[4] WANG Z, SHEN X Q, JING M X,et al. Enhanced arsenic removal from drinking water by FeOOH/γ-Al₂O₃ granules. Journal of Alloys and Compounds, 2018, 735: 1620.
[5] LI R H, JIA Y Z, HU N N.3D hierarchical flower like alumina nanomaterials: preparation and arsenic removal performance.Journal of Inorganic Materials, 2019, 34(5): 553.
[6] ZHOU Z, YU Y Q, DING Z X,et al. Competitive adsorption of arsenic and fluoride on{201}TiO₂. Applied Surface Science, 2019, 466: 425.
[7] DENG M, WU X D, ZHU A M,et al. Well-dispersed TiO₂ nanoparticles anchored on Fe₃O₄ magnetic nanosheets for efficient arsenic removal. Journal of Environmental Management, 2019, 237: 63.
[8] SHEHZAD K, AHMAD M, HE J Y,et al. Synthesis of ultra-large ZrO₂ nanosheets as novel adsorbents for fast and efficient removal of As(III) from aqueous solutions. Journal of Colloid and Interface Science, 2019, 533: 588.
[9] LI R H, YANG W Y, GAO S,et al. Hydrous cerium oxides coated glass fiber for efficient and long-lasting arsenic removal from drinking water. Journal of Advanced Ceramics, 2021, 10(2): 247.
[10] LI R H, LI Q, GAO S A,et al. Exceptional arsenic adsorption performance of hydrous cerium oxide nanoparticles: part A. Adsorption capacity and mechanism. Chemical Engineering Journal, 2012, 185: 127.
[11] ZHANG Y, DOU X M, ZHAO B,et al. Removal of arsenic by a granular Fe-Ce oxide adsorbent: fabrication conditions and performance. Chemical Engineering Journal, 2010, 162(1): 164.
[12] DENG S B, LI Z J, HUANG J,et al. Preparation, characterization and application of a Ce-Ti oxide adsorbent for enhanced removal of arsenate from water. Journal of Hazardous Materials, 2010, 179(1/2/3): 1014.
[13] CHEN J, WANG J Y, ZHANG G S,et al. Facile fabrication of nanostructured cerium-manganese binary oxide for enhanced arsenite removal from water. Chemical Engineering Journal, 2018, 334: 1518.
[14] SUN C Z, QIU J W, ZHANG Z B,et al. Removal of arsenite from water by Ce-Al-Fe trimetal oxide adsorbent: kinetics, isotherms, and thermodynamics. Journal of Chemistry, 2016, 2016: 8617219.
[15] CAMPOS P T A, OLIVEIRA C F, LIMA J P V,et al. Cerium-zirconium mixed oxide synthesized by Sol-Gel method and its effect on the oxygen vacancy and specific surface area. Journal of Solid State Chemistry, 2022, 307: 122752.
[16] TAKAHASHI H, TAKEGUCHI T, YAMAMOTO N,et al. Ni cermet solid oxide fuel cell anodes prepared from nanoparticle Y₂O₃-CeO₂-ZrO₂ solid solutions. Solid State Ionics, 2011, 185(1): 52.
17 [17] AHN K, HE H P, VOHS J M, et al. Enhanced thermal stability of SOFC anodes made with CeO₂-ZrO₂ solutions. Electrochemical and Solid-State Letters, 2005, 8(8): A414.
[18] ZABILSKIY M, MA K B, BECK A,et al. Methanol synthesis over Cu/CeO₂-ZrO₂ catalysts: the key role of multiple active components. Catalysis Science & Technology, 2021, 11(1): 349.
[19] MAIA T A, ASSAF E M.Catalytic features of Ni supported on CeO₂-ZrO₂ solid solution in the steam reforming of glycerol for syngas production.RSC Advances, 2014, 4(59): 31142.
[20] 周益, 赵月昌, 贾嘉, 等. 铈锆铝复合氧化物的制备及其性能研究. 中国稀土学报, 2014, 32(3): 304.
[21] YUAN W H, ZHOU C C, LI L.Study on catalytic properties of nano-CeO₂-ZrO₂ mixed oxides prepared by modified Sol-Gel method.Journal of Inorganic Materials, 2010, 25(8): 820.
[22] THAMMACHART M, MEEYOO V, RISKSOMBOON T,et al. Catalytic activity of CeO₂-ZrO₂ mixed oxide catalysts prepared via Sol-Gel technique: CO oxidation. Catalysis Today, 2001, 68(1/2/3): 53.
[23] 张馥鼎, 马新胜, 高玮. 纳米稀土—锆固溶体的合成及高温稳定性研究. 稀土, 2007, 28(4): 19.
[24] ZHANG Y, YANG M, DOU X M,et al. Arsenate adsorption on an Fe-Ce bimetal oxide adsorbent: role of surface properties. Environmental Science & Technology, 2005, 39(18): 7246.
[25] ZHANG G S, QU J H, LIU H J,et al. Removal mechanism of As(III) by a novel Fe-Mn binary oxide adsorbent: oxidation and sorption. Environmental Science & Technology, 2007, 41(13): 4613.
[26] PENA M, MENG X G, KORFIATIS G P,et al. Adsorption mechanism of arsenic on nanocrystalline titanium dioxide. Environmental Science & Technology, 2006, 40(4): 125

一步醇热法制备纳米CeO₂-ZrO₂固溶体及其除砷性能

One-step Alcohothermal Synthesis of Nanocrystalline CeO₂-ZrO₂ Solid Solution and Its Arsenic Removal Performance

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 3

编辑推荐

Metrics

本文评价

[1]	戴洁燕, 冯爱虎, 米乐, 于洋, 崔苑苑, 于云. NaY沸石分子吸附涂层对典型空间污染物的吸附机制研究[J]. 无机材料学报, 2023, 38(10): 1237-1244.
[2]	董丽佳, 吴思颖, 李生波, 魏作富, 杨国, 胡保卫. 稻草生物炭对铕的吸附行为及机理研究[J]. 无机材料学报, 2020, 35(3): 390-398.
[3]	张俊,王德平,姚爱华,黄文旵. 纳米羟基磷灰石对Ni²⁺的吸附性能及机理研究[J]. 无机材料学报, 2009, 24(2): 269-274.