Advances in Formation Mechanism and Environmental Effects of Charge-assistedHydrogen Bonds
WANG Peng1,2, XIAO Di1,2, LIANG Ni1,2, ZHOU Riyu3, ZHANG Di1,2
1 Faculty of Environmental Science and Engineering, Kunming University of Science & Technology, Kunming 650500; 2 Yunnan Key Laboratory of Carbon Sequestration and Pollution Control, Kunming 650500; 3 School of Environment and Resource, Southwest University of Science and Technology, Mianyang 621010
Abstract: As a common intermolecular interaction force, hydrogen bonds play a significant role in physical, chemical and biological processes. And this so-called “weak interaction” has long been studied extensively. Thanks to its unique orientation and specificity of bonding, hydrogen bonding effect can regulate molecular aggregation perfectly, which has been widely applied in synthesis of crystal materials. Especially, the hydrogen bonds formed with the assist of ion or charge, namely the charge-assisted hydrogen bonds (CAHB), exhibit a binding strength stronger than ordinary hydrogen bond, and equivalent to covalent bond, which has aroused numerous interests of researchers. Different from ordinary hydrogen bonds, there is a charge distribution between the two substances that form the CAHB. Actually, just the distribution of charge in a given resonance structure dominant the formation of the relatively strong CAHB. In addition, there is also Coulomb interaction between the amphoteric ion component and the carrier carrying the opposite charge. The existence of two energy-equivalent valence bond resonance forms result in the stronger binding CAHB. Specifically, (+)CAHB is formed between the positive charge on the proton donor atom; and (-)CAHB is formed between the formal negative charge on the proton accepting group. It has been also found that CAHB, as a kind of low-resistance hydrogen bond or a salt bridge similar to a cation bridge, is ubiquitous in environmental processes. They possess not only bonding strength much stronger than ordinary hydrogen bonds, but also characteristics similar to covalent bonds, which is beneficial to the self-assembly process of many environmental media. The super macromolecular structure formed by CAHB is the main form of natural organic matter (NOM) in the environment. Adsorption is commonly used to remove the dissociable amphoteric organic pollutants in water environments. The electrostatic interaction between carbon-based adsorbents and ionic compounds may be the main adsorption mechanism for the removal of these ionic compounds. However, a number of other studies have noted that individual electrostatic interaction alone is not able to explain the effect of pH on the adsorption of dissociated ionic contaminants. Apparently, there exists additional physical or chemical interaction mechanisms that need to be further investigated. While CAHB can be well used to explain some abnormal phenomena in adsorption experiments, such as the strong interaction between the negatively charged adsorbates and the adsorbents. In this article, the key formation mechanism of CAHB in the environment and their environmental effects are summarized. Combining with some experimental data, the important mechanism of natural organic matter (including humic substances and dissolved organic matter) conjugating and forming supramolecules via CAHB is discussed with emphasis. Finally, the environment behavior of ionic compounds affected by natural organic matter under the complex water quality conditions with the participation of CAHB is mentioned. The selection and preparation of carbon-based adsorbents for the removal of ionic compounds are also suggested.
作者简介: 王朋,2013年6月毕业于昆明理工大学,获得工学硕士学位。目前主要研究领域为碳纳米材料和有机污染物环境行为。张迪,博士,美国University of Massachusetts Amherst博士后,副教授,博士生导师,云南省中青年学术和技术带头人后备人才,2016年云南省自然科学奖二等奖获得者,伍达观教育基金杰出教师奖获得者,享受云南省高层次人才住房和工作经费。其中,2015年破格晋升副教授,2017年破格晋升博士研究生导师。他的研究领域主要包括:Ⅰ.纳米材料的环境行为和风险;Ⅱ.工程纳米材料的环境应用;Ⅲ.真菌的分类和多样性。主持国家基金2项,省部级项目2项。zhangdi2002113@sina.com
引用本文:
王朋, 肖迪, 梁妮, 周日宇, 张迪. 电荷辅助氢键的形成机制及环境效应研究进展[J]. 材料导报, 2019, 33(5): 812-818.
WANG Peng, XIAO Di, LIANG Ni, ZHOU Riyu, ZHANG Di. Advances in Formation Mechanism and Environmental Effects of Charge-assistedHydrogen Bonds. Materials Reports, 2019, 33(5): 812-818.
1 Mahmudov K T, Pombeiro A J. Chemistry-A European Journal,2016,22,16356. 2 Braga D, Grepioni F. Accounts of Chemical Research,2000,33,601. 3 Gilli P, Bertolasi V, Ferretti V, et al. Journal of the American Chemical Society,1994,116,909. 4 Gilli G,Gilli P. The nature of the hydrogen bond, Oxford University Press, UK,2009. 5 Son S U, Reingold J A, Carpenter G B, et al. Organometallics,2006,25,5276. 6 Piccolo A. Advances in agronomy, Elsevier, US,2002. 7 Piccolo A. Humic substances in terrestrial ecosystems, Elsevier, Netherlands,1996. 8 Xie M, Chen W, Xu Z, et al. Environmental Pollution,2014,186,187. 9 Gilli G, Gilli P. Journal of Molecular Structure,2000,552,1. 10 Xiao F, Pignatello J J. Environmental Science & Technology,2016,50,6276. 11 Lehn J M. Supramolecular chemistry, Vch, Weinheim, GER,1995. 12 Adachi K, Sugiyama Y, Yoneda K, et al. Chemistry-A European Journal,2005,11,6616. 13 Prins L J, Reinhoudt D N, Timmerman P. Angewandte Chemie International Edition,2001,40,2382. 14 Arunan E, Desiraju G R, Klein R A, et al. Pure and Applied Chemistry,2011,83,1637. 15 Desiraju G R, Steiner T. International Union of Crystal, Oxford University Press, UK,2001. 16 Sobczyk L, Grabowski S J, Krygowski T M. Chemical Reviews,2005,105,3513. 17 Adams H, Carver F J, Hunter C A, et al. Angewandte Chemie International Edition,1996,35,1542. 18 Corbin P S, Zimmerman S C. Journal of the American Chemical Society,2000,122,3779. 19 Gilli G, Bellucci F, Ferretti V, et al. Journal of the American Chemical Society,1989,111,1023. 20 Gilli P, Bertolasi V, Ferretti V, et al. Journal of the American Chemical Society,1994,116,909. 21 Bankiewicz B, Palusiak M. Computational and Theoretical Chemistry,2011,966,113. 22 Ward M D. Chemical Communications, DOI: 10.1039/b513077h. 23 Schmuck C. Chemical Communications, DOI: 10.1039/A901126I. 24 Braga D, Polito M, Bracaccini M, et al. Organometallics,2003,22,2142. 25 Kononova M M. Soil organic matter: Its nature, its role in soil formation and in soil fertility, Pergamon Press, US,1966. 26 Stevenson F J. Humus chemistry: Genesis, composition, reactions,Wiley, US,1994. 27 Dubach P, Mehta N C. Soils Fertil,1963,26,293. 28 Conte P,Piccolo A. Environmental Science & Technology,1999,33,1682. 29 Piccolo A, Nardi S, Concheri G. European Journal of Soil Science,1996,47,319. 30 Piccolo A, Nardi S, Concheri G. Chemosphere,1996,33,595. 31 Piccolo A, Conte P, Cozzolino A. European Journal of Soil Science,1999,50,687. 32 Cozzolino A, Piccolo A. Soil Biology & Biochemistry,2002,33,563. 33 Zhao J, Chu G, Pan B, et al. Environmental Science & Technology,2018,52,5173. 34 Li X, Pignatello J J, Wang Y, et al. Environmental Science & Technology,2013,47,8334. 35 Franz M, Arafat H A, Pinto N G. Carbon,2000,38,1807. 36 Lian F, Sun B, Song Z, et al. Chemical Engineering Journal,2014,248,128. 37 Moreno-Castilla C. Carbon,2004,42,83. 38 Gilli P, Pretto L, Bertolasi V, et al. Accounts of Chemical Research,2008,42,33. 39 Teixidó M, Pignatello J J, Beltrán J L, et al. Environmental Science & Technology,2011,45,10020. 40 Lee J W, Kidder M, Evans B R, et al. Environmental Science & Techno-logy,2010,44,7970. 41 Silber A, Levkovitch I, Graber E. Environmental Science & Technology,2010,44,9318. 42 Fang Q, Chen B, Lin Y, et al. Environmental Science & Technology,2013,48,279. 43 Li H, Cao Y, Zhang D, et al. Science of the Total Environment,2018,618,269.
渝公网安备50019002502923号 版权所有：《材料导报》编辑部
2019, Vol. 33 
