PMID- 35868019 OWN - NLM STAT- MEDLINE DCOM- 20221111 LR - 20230120 IS - 1936-086X (Electronic) IS - 1936-0851 (Print) IS - 1936-0851 (Linking) VI - 16 IP - 8 DP - 2022 Aug 23 TI - Tailoring Diffusional Fields in Zwitterion/Dopamine Copolymer Electropolymerized at Carbon Nanowalls for Sensitive Recognition of Neurotransmitters. PG - 13183-13198 LID - 10.1021/acsnano.2c06406 [doi] AB - The importance of neurotransmitter sensing in the diagnosis and treatment of many psychological illnesses and neurodegenerative diseases is non-negotiable. For electrochemical sensors to become widespread and accurate, a long journey must be undertaken for each device, from understanding the materials at the molecular level to real applications in biological fluids. We report a modification of diamondized boron-doped carbon nanowalls (BCNWs) with an electropolymerized polydopamine/polyzwitterion (PDA|PZ) coating revealing tunable mechanical and electrochemical properties. Zwitterions are codeposited with PDA and noncovalently incorporated into a structure. This approach causes a specific separation of the diffusion fields generated by each nanowall during electrochemical reactions, thus increasing the contribution of the steady-state currents in the amperometric response. This phenomenon has a profound effect on the sensing properties, leading to a 4-fold enhancement of the sensitivity (3.1 to 14.3 muA cm(-2) muM(-1)) and a 5-fold decrease of the limit of detection (505 to 89 nM) in comparison to the pristine BCNWs. Moreover, as a result of the antifouling capabilities of the incorporated zwitterions, this enhancement is preserved in bovine serum albumin (BSA) with a high protein concentration. The presence of zwitterion facilitates the transport of dopamine in the direction of the electrode by intermolecular interactions such as cation-pi and hydrogen bonds. On the other hand, polydopamine units attached to the surface form molecular pockets driven by hydrogen bonds and pi-pi interactions. As a result, the intermediate state of dopamine-analyte oxidation is stabilized, leading to the enhancement of the sensing properties. FAU - Olejnik, Adrian AU - Olejnik A AD - Department of Metrology and Optoelectronics, Faculty of Electronics, Telecommunications and Informatics, Gdansk University of Technology, Narutowicza 11/12 St., 80-233 Gdansk, Poland. AD - Centre for Plasma and Laser Engineering, The Szewalski Institute of Fluid-Flow Machinery, Polish Academy of Sciences, Fiszera 14 St., 80-231 Gdansk, Poland. FAU - Ficek, Mateusz AU - Ficek M AUID- ORCID: 0000-0003-2334-9697 AD - Department of Metrology and Optoelectronics, Faculty of Electronics, Telecommunications and Informatics, Gdansk University of Technology, Narutowicza 11/12 St., 80-233 Gdansk, Poland. FAU - Szkodo, Marek AU - Szkodo M AD - Institute of Manufacturing and Materials Technology, Faculty of Mechanical Engineering and Ship Technology, Gdansk University of Technology, Narutowicza 11/12 St., 80-233 Gdansk, Poland. FAU - Stanislawska, Alicja AU - Stanislawska A AD - Institute of Manufacturing and Materials Technology, Faculty of Mechanical Engineering and Ship Technology, Gdansk University of Technology, Narutowicza 11/12 St., 80-233 Gdansk, Poland. FAU - Karczewski, Jakub AU - Karczewski J AD - Institute of Nanotechnology and Materials Engineering and Advanced Materials Center, Gdansk University of Technology, Narutowicza 11/12, 80-233 Gdansk, Poland. FAU - Ryl, Jacek AU - Ryl J AUID- ORCID: 0000-0002-0247-3851 AD - Institute of Nanotechnology and Materials Engineering and Advanced Materials Center, Gdansk University of Technology, Narutowicza 11/12, 80-233 Gdansk, Poland. FAU - Dolega, Anna AU - Dolega A AUID- ORCID: 0000-0003-0509-2285 AD - Department of Inorganic Chemistry, Faculty of Chemistry, Gdansk University of Technology, Narutowicza 11/12 St., 80-233 Gdansk, Poland. FAU - Siuzdak, Katarzyna AU - Siuzdak K AUID- ORCID: 0000-0001-7434-6408 AD - Centre for Plasma and Laser Engineering, The Szewalski Institute of Fluid-Flow Machinery, Polish Academy of Sciences, Fiszera 14 St., 80-231 Gdansk, Poland. FAU - Bogdanowicz, Robert AU - Bogdanowicz R AUID- ORCID: 0000-0002-7543-2620 AD - Department of Metrology and Optoelectronics, Faculty of Electronics, Telecommunications and Informatics, Gdansk University of Technology, Narutowicza 11/12 St., 80-233 Gdansk, Poland. LA - eng PT - Journal Article PT - Research Support, Non-U.S. Gov't DEP - 20220722 PL - United States TA - ACS Nano JT - ACS nano JID - 101313589 RN - VTD58H1Z2X (Dopamine) RN - 7440-44-0 (Carbon) RN - 0 (Neurotransmitter Agents) SB - IM MH - *Dopamine MH - *Carbon/chemistry MH - Electrochemical Techniques MH - Electrodes MH - Neurotransmitter Agents PMC - PMC9413423 OTO - NOTNLM OT - carbon nanowalls OT - coelectropolymerization OT - diffusion fields OT - nanoindentation OT - polydopamine OT - sensing OT - zwitterions COIS- The authors declare no competing financial interest. EDAT- 2022/07/23 06:00 MHDA- 2022/11/15 06:00 PMCR- 2022/08/26 CRDT- 2022/07/22 16:53 PHST- 2022/07/23 06:00 [pubmed] PHST- 2022/11/15 06:00 [medline] PHST- 2022/07/22 16:53 [entrez] PHST- 2022/08/26 00:00 [pmc-release] AID - 10.1021/acsnano.2c06406 [doi] PST - ppublish SO - ACS Nano. 2022 Aug 23;16(8):13183-13198. doi: 10.1021/acsnano.2c06406. Epub 2022 Jul 22.