PMID- 28397501 OWN - NLM STAT- MEDLINE DCOM- 20190109 LR - 20240327 IS - 1944-8252 (Electronic) IS - 1944-8244 (Print) IS - 1944-8244 (Linking) VI - 9 IP - 17 DP - 2017 May 3 TI - Layer-by-Layer-Assembled Laccase Enzyme on Stimuli-Responsive Membranes for Chloro-Organics Degradation. PG - 14858-14867 LID - 10.1021/acsami.7b01999 [doi] AB - Functionalized membranes provide versatile platforms for the incorporation of biocatalysts and nanostructured materials for efficient and benign environmental remediation. The existing techniques for remediating chloro-organics in water consist of both physical and chemical means mostly using metal oxide-based catalysts, despite associated environmental concerns. To offer bioinspired remediation as an alternative, we herein demonstrate a layer-by-layer approach to immobilize laccase enzyme onto pH-responsive functionalized membranes for the degradation of chloro-organics in water. The efficacy of these bioinspired membranes toward dechlorination of 2,4,6-trichlorophenol (TCP) is demonstrated under a pressure-driven continuous flow mode (convective flow) for the first time to the best of our knowledge. Over 80% of the initial TCP was degraded at an optimum flow rate under an applied air pressure of about 0.7 bar or lower. This corresponds to degradation of a substantial amount of the initial substrate in only 36 s residence time, whereas it takes hours for degradation in a batch reaction. This, in fact, demonstrates an energy efficient flow-through system with potentially large-scale applications. Comparison of the stability of the enzyme in the solution phase versus immobilized on the membrane phase showed a loss of some 65% of enzyme activity in the solution phase after 22 d, whereas the membrane-bound enzyme lost only a negligible percentage of the activity in a comparable time span. Finally, the membrane was exposed to rigorous cycles of TCP degradation trials to study its reusability. The primary results reveal a loss of only 14% of the initial activity after 4 cycles of use in a period of 25 d, demonstrating its potential to be reused. Regeneration of the functionalized membrane was also validated by dislodging the immobilized enzyme, followed by immobilization of fresh enzyme onto the membrane. FAU - Sarma, Rupam AU - Sarma R AUID- ORCID: 0000-0003-3539-5949 AD - Department of Chemical and Materials Engineering, University of Kentucky , 177 F. Paul Anderson Tower, Lexington, Kentucky 40506, United States. FAU - Islam, Md Saiful AU - Islam MS AD - Department of Chemical and Materials Engineering, University of Kentucky , 177 F. Paul Anderson Tower, Lexington, Kentucky 40506, United States. FAU - Miller, Anne-Frances AU - Miller AF AD - Department of Chemical and Materials Engineering, University of Kentucky , 177 F. Paul Anderson Tower, Lexington, Kentucky 40506, United States. FAU - Bhattacharyya, Dibakar AU - Bhattacharyya D AUID- ORCID: 0000-0001-9948-9085 AD - Department of Chemical and Materials Engineering, University of Kentucky , 177 F. Paul Anderson Tower, Lexington, Kentucky 40506, United States. LA - eng GR - P42 ES007380/ES/NIEHS NIH HHS/United States PT - Journal Article DEP - 20170421 PL - United States TA - ACS Appl Mater Interfaces JT - ACS applied materials & interfaces JID - 101504991 RN - 0 (Chlorophenols) RN - 0 (Enzymes, Immobilized) RN - EC 1.10.3.2 (Laccase) SB - IM MH - Chlorophenols MH - Enzyme Stability MH - Enzymes, Immobilized MH - Laccase/*metabolism MH - Membranes PMC - PMC5787852 MID - NIHMS936573 OTO - NOTNLM OT - catalysis OT - enzyme immobilization OT - functionalized membrane OT - laccase OT - layer-by-layer assembly OT - trichlorophenol EDAT- 2017/04/12 06:00 MHDA- 2019/01/10 06:00 PMCR- 2018/05/03 CRDT- 2017/04/12 06:00 PHST- 2017/04/12 06:00 [pubmed] PHST- 2019/01/10 06:00 [medline] PHST- 2017/04/12 06:00 [entrez] PHST- 2018/05/03 00:00 [pmc-release] AID - 10.1021/acsami.7b01999 [doi] PST - ppublish SO - ACS Appl Mater Interfaces. 2017 May 3;9(17):14858-14867. doi: 10.1021/acsami.7b01999. Epub 2017 Apr 21.