Carboxyl functionalization and reverse osmosis performance of ethenylene-bridged organosilica membranes

XU Rong; CHENG Xu; DENG Song; QI Lyu; REN Xiuxiu; ZHANG Qi; ZHONG Jing

doi:10.11949/0438-1157.20190078

您当前的位置：

首页 >

文章列表页 >

Carboxyl functionalization and reverse osmosis performance of ethenylene-bridged organosilica membranes

Material science and engineering\, nanotechnology | 更新时间：2026-07-24

- Carboxyl functionalization and reverse osmosis performance of ethenylene-bridged organosilica membranes
- CIESC Journal Vol. 70, Issue 7, Pages: 2766-2774(2019)
- 作者机构：
  
  常州大学石油化工学院，江苏省绿色催化材料与技术重点实验室，江苏常州 213164
- 作者简介：
- 基金信息：
- DOI：10.11949/0438-1157.20190078
  CLC： TQ 028
- Received：25 January 2019，
  
  Revised：2019-04-10，
  
  Online First：24 July 2026，
  
  Published：05 July 2019
- 稿件说明：
移动端阅览
徐荣, 程旭, 邓松, 戚律, 任秀秀, 张琪, 钟璟. 乙烯基桥联有机硅膜的羧基化改性及反渗透性能研究[J]. 化工学报, 2019, 70(7): 2766-2774

XU Rong, CHENG Xu, DENG Song, QI Lyu, REN Xiuxiu, ZHANG Qi, ZHONG Jing. Carboxyl functionalization and reverse osmosis performance of ethenylene-bridged organosilica membranes[J]. CIESC Journal, 2019, 70(7): 2766-2774
徐荣, 程旭, 邓松, 戚律, 任秀秀, 张琪, 钟璟. 乙烯基桥联有机硅膜的羧基化改性及反渗透性能研究[J]. 化工学报, 2019, 70(7): 2766-2774 DOI： 10.11949/0438-1157.20190078.

XU Rong, CHENG Xu, DENG Song, QI Lyu, REN Xiuxiu, ZHANG Qi, ZHONG Jing. Carboxyl functionalization and reverse osmosis performance of ethenylene-bridged organosilica membranes[J]. CIESC Journal, 2019, 70(7): 2766-2774 DOI： 10.11949/0438-1157.20190078.

摘要

利用1

2-二(三乙氧基硅基)乙烯(BTESEthy)和硫代苹果酸(MSA)的巯基-烯点击反应对桥联有机硅进行羧基化改性，以管式α-Al

微滤膜为支撑体制备羧基官能化的桥联有机硅膜。通过傅里叶变换红外光谱(FT-IR)、激光粒度仪(DLS)、智能重量分析仪(IGA)和扫描电镜(SEM)等对膜结构和表面性质进行了表征。量子化学计算表明羧基化改性的有机硅网络拥有更加致密的孔结构和更高的水亲和力。将改性的BTESEthy-MSA膜用于反渗透脱盐，系统考察了BTESEthy-MSA膜反渗透脱盐性能。实验结果表明，与BTESEthy膜相比，羧基化改性的BTESEthy-MSA膜的水渗透率和盐截留率均有所提高。同时，BTESEthy-MSA膜表现出优异的水热稳定性和耐氯性能。在250 h的长期反渗透测试中，BTESEthy-MSA膜的水渗透率高达3.2×10

-13

/(m

·s·Pa)，NaCl截留率始终保持在94.7%以上。

Abstract

Carboxyl functionalized bridged-type organosilica membranes were prepared

via

the thiol-ene click reaction between 1

2-bis(triethoxysilyl)ethylene (BTESEthy) and mercaptosuccinic acid (MSA)

using tubular α-Al

microfiltration membranes as the supports. The membrane structure and surface properties were characterized by Fourier transform infrared spectroscopy (FT-IR)

dynamic light scattering (DLS)

intelligent gravimetric analyzer (IGA) and scanning electron microscopy (SEM). Quantum chemistry calculations show that the carboxylated modified silicone network has a denser pore structure and higher water affinity. The prepared BTESEthy-MSA membranes were applied to desalination by reverse osmosis. The reverse osmosis performance of BTESEthy-MSA membranes was systematically investigated. The experimental results showed that compared with the original BTESEthy membranes

both water permeability and salt rejection of the carboxyl functionalized BTESEthy-MSA membranes were improved. Meanwhile

the BTESEthy-MSA membranes exhibit superior hydrothermal stability and chlorine resistance. Moreover

the BTESEthy-MSA membranes exhibited high stability over long term reverse osmosis test of 250 h

and high water permeability of 3.2×10

-13

/(m

·s·Pa) and NaCl rejections of

94.7%.

关键词

Keywords

references

张雪杰 , 李亮 , 蔡志强 , 等 . 改性化合物对聚酰胺膜材料亲水性及抗污染性能影响的分子力学计算与实验研究 [J ] . 化工学报 , 2012 , 63 ( 6 ): 1957 - 1966 .

Zhang X J , Li L , Cai Z Q , et al . Effects of modification chemical on hydrophilic and antifouling properties of polyamide membranes：molecular mechanics calculation and experimental investigation [J ] . CIESC Journal , 2012 , 63 ( 6 ): 1957 - 1966 .

潘春佑 , 徐国荣 , 李露 , 等 . 聚酰胺反渗透复合膜改性技术研究进展 [J ] . 膜科学与技术 , 2016 , 36 ( 6 ): 133 - 138 .

Pan C Y , Xu G R , Li L , et al . Developments and perspectives on the polyamide-based reverse osmosis desalination membranes [J ] . Membrane Science and Technology , 2016 , 36 ( 6 ): 133 - 138 .

Gutman J , Herzberg M , Walker S L . Biofouling of reverse osmosis membranes: positively contributing factors of sphingomonas [J ] . Environmental Science & Technology , 2014 , 48 ( 23 ): 13941 - 13950 .

Castricum H L , Sah A , Kreiter R , et al . Hydrothermally stable molecular separation membranes from organically linked silica [J ] . Journal of Materials Chemistry , 2008 , 18 ( 18 ): 2150 - 2158 .

Castricum H L , Sah A , Kreiter R , et al . Hybrid ceramic nanosieves: stabilizing nanopores with organic links [J ] . Chemical Communications , 2008 , ( 9 ): 1103 - 1105 .

Kanezashi M , Yada K , Yoshioka T , et al . Design of silica networks for development of highly permeable hydrogen separation membranes with hydrothermal stability [J ] . Journal of the American Chemical Society , 2009 , 131 ( 2 ): 414 - 415 .

Kanezashi M , Yada K , Yoshioka T , et al . Organic-inorganic hybrid silica membranes with controlled silica network size: preparation and gas permeation characteristics [J ] . Journal of Membrane Science , 2010 , 348 ( 1 ): 310 - 318 .

漆虹 , 韩静 , 江晓骆 , 等 . 有机-无机复合SiO 2 膜的制备及水蒸气稳定性能研究 [J ] . 无机材料学报 , 2010 , 25 ( 7 ): 758 - 764 .

Qi H , Han J , Jiang X L , et al . Preparation and hydrothermal stability of organic-inorganic hybrid silica membrane [J ] . Journal of Inorganic Materials , 2010 , 25 ( 7 ): 758 - 764 .

Qi H , Han J , Xu N , et al . Hybrid organic-inorganic microporous membranes with high hydrothermal stability for the separation of carbon dioxide [J ] . ChemSusChem , 2010 , 3 ( 12 ): 1375 - 1378 .

Xu R , Wang J H , Kanezashi M , et al . Development of robust organosilica membranes for reverse osmosis [J ] . Langmuir , 2011 , 27 ( 23 ): 13996 - 13999 .

Xu R , Kanezashi M , Yoshioka T , et al . Tailoring the affinity of organosilica membranes by introducing polarizable ethenylene bridges and aqueous ozone modification [J ] . ACS Applied Materials & Interfaces , 2013 , 5 ( 13 ): 6147 - 6154 .

Xu R , Ibrahim S M , Kanezashi M , et al . New insights into the microstructure-separation properties of organosilica membranes with ethane, ethylene, and acetylene bridges [J ] . ACS Applied Materials & Interfaces , 2014 , 6 ( 12 ): 9357 - 9364 .

Yamamoto K , Ohshita J , Mizumo T , et al . Preparation of hydroxyl group containing bridged organosilica membranes for water desalination [J ] . Separation and Purification Technology , 2015 , 156 : 396 - 402 .

胡笛 , 徐彩虹 . 巯基-乙烯基加成反应合成含硅聚合物的研究进展 [J ] . 高分子通报 , 2011 , ( 10 ): 111 - 118 .

Hu D , Xu C H . Research progress of silicon containing polymers by thiol-ene chemistry [J ] . Polymer Bulletin , 2011 , ( 10 ): 111 - 118 .

吴建兵 , 凌丽霞 , 马国章 , 等 . 巯基-乙烯基点击反应在紫外光固化过程中的应用 [J ] . 高分子材料科学与工程 , 2013 , 29 ( 10 ): 169 - 174 .

Wu J B , Ling L X , Ma G Z , et al . The application of thiol-ene click reaction in UV curing process [J ] . Polymer Materials Science & Engineering , 2013 , 29 ( 10 ): 169 - 174 .

Asaeda M , Yang J , Sakou Y . Porous silica-zirconia (50%) membranes for pervaporation of iso-propyl alcohol (IPA)/water mixtures [J ] . Journal of Chemical Engineering of Japan , 2002 , 35 ( 4 ): 365 - 371 .

Xu R , Wang J , Kanezashi M , et al . Reverse osmosis performance of organosilica membranes and comparison with the pervaporation and gas permeation properties [J ] . AIChE Journal , 2013 , 59 ( 4 ): 1298 - 1307 .

Han Y H , Taylor A , Mantle M D , et al . Sol-gel-derived organic-inorganic hybrid materials [J ] . Journal of Non-Crystalline Solids , 2007 , 353 ( 3 ): 313 - 320 .

Esquivel D , Canck E D , Jimenez-Sanchidrian C , et al . Formation and functionalization of surface Diels-Alder adducts on ethenylene-bridged periodic mesoporous organosilica [J ] . Journal of Materials Chemistry , 2011 , 21 ( 29 ): 10990 - 10998 .

Sasidharan M , Bhaumik A . Novel and mild synthetic strategy for the sulfonic acid functionalization in periodic mesoporous ethenylene-silica [J ] . ACS Applied Materials & Interfaces , 2013 , 5 ( 7 ): 2618 - 2625 .

Yamamoto K , Ohshita J , Mizumo T , et al . Synthesis of organically bridged trialkoxysilanes bearing acetoxymethyl groups and applications to reverse osmosis membranes: acetoxymethyl-containing bridged silica membrane [J ] . Applied Organometallic Chemistry , 2016 , 31 ( 3 ): e3580 .

Thommes M , Morell J , Cychosz K A , et al . Combining nitrogen, argon, and water adsorption for advanced characterization of ordered mesoporous carbons (CMKs) and periodic mesoporous organosilicas (PMOs) [J ] . Langmuir , 2013 , 29 ( 48 ): 14893 - 14902 .

Fan C , Nguyen V , Zeng Y , et al . Novel approach to the characterization of the pore structure and surface chemistry of porous carbon with Ar, N 2 , H 2 O and CH 3 OH adsorption [J ] . Microporous and Mesoporous Materials , 2015 , 209 : 79 - 89 .

Ibrahim S M , Nagasawa H , Kanezashi M , et al . Organosilica bis(triethoxysilyl)ethane (BTESE) membranes for gas permeation (GS) and reverse osmosis (RO): the effect of preparation conditions on structure, and the correlation between gas and liquid permeation properties [J ] . Journal of Membrane Science , 2017 , 526 : 242 - 251 .

Geise G M , Park H B , Sagle A C , et al . Water permeability and water/salt selectivity trade off in polymers for desalination [J ] . Journal of Membrane Science , 2011 , 369 ( 1 / 2 ): 130 - 138 .

Xu R , Lin P , Zhang Q , et al . Development of ethenylene-bridged organosilica membranes for desalination applications [J ] . Industrial & Engineering Chemistry Research , 2016 , 55 ( 7 ): 2183 - 2190 .

Park H , Freeman B , Zhang Z B , et al . Highly chlorine-tolerant polymers for desalination [J ] . Angewandte Chemie International Edition , 2010 , 47 ( 32 ): 6019 - 6024 .

Hatakeyama E S , Gabriel C J , Wiesenauer B R , et al . Water filtration performance of a lyotropic liquid crystal polymer membrane with uniform, sub-1-nm pores [J ] . Journal of Membrane Science , 2011 , 366 ( 1 / 2 ): 62 - 72 .

Kiso Y , Muroshige K , Oguchi T , et al . Pore radius estimation based on organic solute molecular shape and effects of pressure on pore radius for a reverse osmosis membrane [J ] . Journal of Membrane Science , 2011 , 369 ( 1 / 2 ): 290 - 298 .

Li L X , Liu N , McPherson B , et al . Enhanced water permeation of reverse osmosis through MFI-type zeolite membranes with high aluminum contents [J ] . Industrial & Engineering Chemistry Research , 2007 , 46 ( 5 ): 1584 - 1589 .

Antony A , Fudianto R , Cox S , et al . Assessing the oxidative degradation of polyamide reverse osmosis membrane-accelerated ageing with hypochlorite exposure [J ] . Journal of Membrane Science , 2010 , 347 ( 1 / 2 ): 159 - 164 .

Views

下载量

CSCD

Alert me when the article has been cited

提交

Tools

Publicity Resources

Forward-osmosis strategy and chemical cleaning of seawater desalination reverse osmosis membranes

Molecular dynamics study of ion rejection process based on Janus nanochannel

Preparation of polyionic liquid membrane and its application in low-sodium and high-potassium healthy soy sauce

Preparation of anti-biofouling reverse osmosis membrane by surface modification with quorum sensing inhibitor

Tailoring preparation of graphene quantum dot composite membranes: influence of precursors

Related Author

TAN Ming

WANG Wenguang

ZHANG Xiaodong

ZHAO Hongwu

ZHANG Yang

YANG Xingtao

LI Zirui

QI Kai

Related Institution

College of Environment and Safety Engineering, Qingdao University of Science & Technology

Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences

Qingdao Befesa Seawater Desalination Co. Ltd.

Beijing Key Laboratory of Heat Transfer and Energy Conversion, Beijing University of Technology

College of Environment and Safety Engineering, Qingdao University of Science and Technology

⁰