Energetically efficient electrochemically tunable affinity separation using multicomponent polymeric nanostructures for water treatment

We describe a water treatment strategy, electrochemically tunable affinity separation (ETAS), which, unlike other previously developed electrochemical processes, targets uncharged organic pollutants in water. Key to achieving ETAS resides in the development of multicomponent polymeric nanostructures that simultaneously exhibit the following characteristics: an oxidation-state dependent affinity towards neutral organics, high porosity for sufficient adsorption capacity, and high conductivity to permit electrical manipulation. A prototype ETAS adsorbent composed of nanostructured binary polymeric surfaces that can undergo an electrically-induced hydrophilic–hydrophobic transition can provide programmable control of capture and release of neutral organics in a cyclic fashion. A quantitative energetic analysis of ETAS offers insights into the tradeoff between energy cost and separation extent through manipulation of electrical swing conditions. We also introduce a generalizable materials design approach to improve the separation degree and energetic efficiency simultaneously, and identify the critical factors responsible for such enhancement via redox electrode simulations and theoretical calculations of electron transfer kinetics. The effect of operation mode and multistage configuration on ETAS performance is examined, highlighting the practicality of ETAS and providing useful guidelines for its operation at large scale. The ETAS approach is energetically efficient, environmentally friendly, broadly applicable to a wide range of organic contaminants of various molecular structures, hydrophobicity and functionality, and opens up new avenues for addressing the urgent, global challenge of water purification and wastewater management.

[1]  T. A. Hatton,et al.  Superhydrophobic, Surfactant‐doped, Conducting Polymers for Electrochemically Reversible Adsorption of Organic Contaminants , 2018, Advanced Functional Materials.

[2]  S. Darling,et al.  Crises and opportunities at the energy-water interface , 2018, MRS Bulletin.

[3]  Timothy F. Jamison,et al.  Asymmetric Faradaic systems for selective electrochemical separations , 2017 .

[4]  R. Luque,et al.  Ni-based bimetallic heterogeneous catalysts for energy and environmental applications , 2016 .

[5]  S. Haigh,et al.  Self-catalytic membrane photo-reactor made of carbon nitride nanosheets† , 2016 .

[6]  Ryan P. Lively,et al.  Seven chemical separations to change the world , 2016, Nature.

[7]  Tong Lin,et al.  Fluorine-Free Superhydrophobic Coatings with pH-induced Wettability Transition for Controllable Oil-Water Separation. , 2016, ACS applied materials & interfaces.

[8]  T. A. Hatton,et al.  Enhanced Redox Transformation Efficiency in Unconjugated Electroactive Polymer/Carbon Nanotube Hybrids , 2016 .

[9]  William R. Dichtel,et al.  Rapid removal of organic micropollutants from water by a porous β-cyclodextrin polymer , 2015, Nature.

[10]  Renyuan Li,et al.  Rational design of nanomaterials for water treatment. , 2015, Nanoscale.

[11]  T. A. Hatton,et al.  Electrochemically Nanostructured Polyvinylferrocene/Polypyrrole Hybrids with Synergy for Energy Storage , 2015 .

[12]  Volker Presser,et al.  Water desalination via capacitive deionization : What is it and what can we expect from it? , 2015 .

[13]  Yen Wei,et al.  CO2 -Responsive Nanofibrous Membranes with Switchable Oil/Water Wettability. , 2015, Angewandte Chemie.

[14]  Masahiro Fujiwara,et al.  Photo Induced Membrane Separation for Water Purification and Desalination Using Azobenzene Modified Anodized Alumina Membranes. , 2015, ACS nano.

[15]  K. Lu,et al.  Metal‐Organic Framework Templated Inorganic Sorbents for Rapid and Efficient Extraction of Heavy Metals , 2014, Advanced materials.

[16]  Xiaogang Hao,et al.  A novel potential-responsive ion exchange film system for heavy metal removal , 2014 .

[17]  T. Sultana,et al.  Redox-induced ion pairing of anionic surfactants with ferrocene-terminated self-assembled monolayers: Faradaic electrochemistry and surfactant aggregation at the monolayer/liquid interface. , 2013, Journal of the American Chemical Society.

[18]  Patrick Couvreur,et al.  Stimuli-responsive nanocarriers for drug delivery. , 2013, Nature materials.

[19]  C. Prasse,et al.  Is biological treatment a viable alternative for micropollutant removal in drinking water treatment processes? , 2013, Water research.

[20]  T. A. Hatton,et al.  Metallocene/carbon hybrids prepared by a solution process for supercapacitor applications , 2013 .

[21]  D. Kuckling,et al.  Responsive hydrogels--structurally and dimensionally optimized smart frameworks for applications in catalysis, micro-system technology and material science. , 2013, Chemical Society reviews.

[22]  G. Rutledge,et al.  Polyvinylferrocene for noncovalent dispersion and redox-controlled precipitation of carbon nanotubes in nonaqueous media. , 2013, Langmuir : the ACS journal of surfaces and colloids.

[23]  Paloma Alonso-Magdalena,et al.  Endocrine disruptors in the etiology of type 2 diabetes mellitus , 2011, Nature Reviews Endocrinology.

[24]  T. A. Hatton,et al.  Redox-responsive gels with tunable hydrophobicity for controlled solubilization and release of organics. , 2011, ACS applied materials & interfaces.

[25]  A. Bodour,et al.  Prioritizing research for trace pollutants and emerging contaminants in the freshwater environment. , 2010, Environmental pollution.

[26]  B. K. Dutta,et al.  On separation efficiency , 2010 .

[27]  Stephen M Rappaport,et al.  Environment and Disease Risks , 2010, Science.

[28]  C. Sonnenschein,et al.  Environmental causes of cancer: endocrine disruptors as carcinogens , 2010, Nature Reviews Endocrinology.

[29]  Sung Jae Kim,et al.  Direct seawater desalination by ion concentration polarization. , 2010, Nature nanotechnology.

[30]  M. C. Stuart,et al.  Emerging applications of stimuli-responsive polymer materials. , 2010, Nature materials.

[31]  Xin Li,et al.  Effective removal of rhodamine B from contaminated water using non-covalent imprinted microspheres designed by computational approach. , 2009, Biosensors & bioelectronics.

[32]  J. Georgiadis,et al.  Science and technology for water purification in the coming decades , 2008, Nature.

[33]  Karen A Kidd,et al.  Collapse of a fish population after exposure to a synthetic estrogen , 2007, Proceedings of the National Academy of Sciences.

[34]  R. Schwarzenbach,et al.  The Challenge of Micropollutants in Aquatic Systems , 2006, Science.

[35]  K. Sei,et al.  Biodegradation of a variety of bisphenols under aerobic and anaerobic conditions. , 2006, Water science and technology : a journal of the International Association on Water Pollution Research.

[36]  W. Arnold,et al.  Aqueous photochemistry of triclosan: Formation of 2,4‐dichlorophenol, 2,8‐dichlorodibenzo‐p‐dioxin, and oligomerization products , 2005, Environmental toxicology and chemistry.

[37]  S. Creager,et al.  INTERFACIAL SOLVATION AND DOUBLE-LAYER EFFECTS ON REDOX REACTIONS IN ORGANIZED ASSEMBLIES , 1994 .

[38]  J. Lazorchak,et al.  Concentrations of prioritized pharmaceuticals in effluents from 50 large wastewater treatment plants in the US and implications for risk estimation. , 2014, Environmental pollution.

[39]  A. Nadal Obesity: Fat from plastics? Linking bisphenol A exposure and obesity , 2013, Nature Reviews Endocrinology.

[40]  Ronald W. Rousseau,et al.  Handbook Of Separation Process Technology , 2008 .