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Article ; Online: A Single-Entity Method for Actively Controlled Nucleation and High-Quality Protein Crystal Synthesis

Yang, Ruoyu / Kvetny, Maksim / Brown, Warren / Ogbonna, Edwin N. / Wang, Gangli

Analytical Chemistry. 2023 May 27, v. 95, no. 25 p.9462-9470

2023

Abstract: Lack of controls and understanding in nucleation, which proceeds crystal growth and other phase transitions, has been a bottleneck challenge in chemistry, materials, biology, and other fields. The exemplary needs for better methods for biomacromolecule ... ...

Abstract	Lack of controls and understanding in nucleation, which proceeds crystal growth and other phase transitions, has been a bottleneck challenge in chemistry, materials, biology, and other fields. The exemplary needs for better methods for biomacromolecule crystallization include (1) synthesizing crystals for high-resolution structure determinations in fundamental research and (2) tuning the crystal habit and thus the corresponding properties in materials and pharmaceutical applications. Herein, a deterministic method is established capable of sustaining the nucleation and growth of a single crystal using the protein lysozyme as a prototype. The supersaturation is localized at the interface between a sample and a precipitant solution, spatially confined by the tip of a single nanopipette. The exchange of matter between the two solutions determines the supersaturation, which is controlled by electrokinetic ion transport driven by an external potential waveform. Nucleation and subsequent crystal growth disrupt the ionic current limited by the nanotip and are detected. The nucleation and growth of individual single crystals are measured in real time. Electroanalytical and optical signatures are elucidated as feedbacks with which active controls in crystal quality and method consistency are achieved: five out of five crystals diffract at a true atomic resolution of up to 1.2 Å. As controls, those synthesized under less optimized conditions diffract poorly. The crystal habits during the growth process are tuned successfully by adjusting the flux. The universal mechanism of nano-transport kinetics, together with the correlations of the diffraction quality and crystal habit with the crystallization control parameters, lay the foundation for the generalization to other materials systems.
Keywords	analytical chemistry ; crystallization ; lysozyme ; prototypes
Language	English
Dates of publication	2023-0527
Size	p. 9462-9470.
Publishing place	American Chemical Society
Document type	Article ; Online
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.3c00175
Database	NAL-Catalogue (AGRICOLA)

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Article: Higher Ion Selectivity with Lower Energy Usage Promoted by Electro-osmotic Flow in the Transport through Conical Nanopores

Brown, Warren / Kvetny, Maksim / Yang, Ruoyu / Wang, Gangli

Journal of physical chemistry. 2021 Feb. 03, v. 125, no. 6

2021

Abstract: The tradeoff between selectivity and throughput presents fundamental challenges to improve desalination and charge storage, salinity gradient-based energy harvesting, memory device/circuit development, and so forth. The well-known ion-current ... ...

Abstract	The tradeoff between selectivity and throughput presents fundamental challenges to improve desalination and charge storage, salinity gradient-based energy harvesting, memory device/circuit development, and so forth. The well-known ion-current rectification and the recently resolved time-dependent transport hysteresis in conical nanopores or asymmetric nanointerfaces offer new opportunities for the selective transport of matter. This report shows that electro-osmotic flow (EOF) is an overlooked factor that increases ion selectivity while maintaining enhanced transport throughput in rectified nanoscale electrokinetic transport. The increased selectivity originates primarily from the suppression of anion flux by the fluid flow in the opposite direction under the applied electrical field. By solving the Poisson and Nernst–Planck (PNP) equations without and with coupled Navier–Stokes (PNP–NS) equations, the EOF effects on cation and anion transport are unequivocally revealed in asymmetric nanopipettes. The flux of cations and anions as well as the transference number and flow velocity are elucidated using the models and boundary conditions validated by previous experiments. A dimensionless parameter, radius over the Debye length, reveals optimal ion selectivity and energy cost at intermediate ion concentrations and nanopore sizes, up to hundreds of millimolars and tens of nanometers under time-dependent potential stimulus. The fundamental insights into EOF at nanointerfaces suggest new routes/strategies for better separation, analysis, and energy applications.
Keywords	cations ; desalination ; electric field ; electroosmosis ; energy ; energy costs ; hysteresis ; nanopores ; salinity
Language	English
Dates of publication	2021-0203
Size	p. 3269-3276.
Publishing place	American Chemical Society
Document type	Article
Note	NAL-AP-2-clean
ISSN	1932-7455
DOI	10.1021/acs.jpcc.0c08863
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: A Single-Entity Method for Actively Controlled Nucleation and High-Quality Protein Crystal Synthesis.

Yang, Ruoyu / Kvetny, Maksim / Brown, Warren / Ogbonna, Edwin N / Wang, Gangli

Analytical chemistry

2023 Volume 95, Issue 25, Page(s) 9462–9470

Abstract	Lack of controls and understanding in nucleation, which proceeds crystal growth and other phase transitions, has been a bottleneck challenge in chemistry, materials, biology, and other fields. The exemplary needs for better methods for biomacromolecule crystallization include (1) synthesizing crystals for high-resolution structure determinations in fundamental research and (2) tuning the crystal habit and thus the corresponding properties in materials and pharmaceutical applications. Herein, a deterministic method is established capable of sustaining the nucleation and growth of a single crystal using the protein lysozyme as a prototype. The supersaturation is localized at the interface between a sample and a precipitant solution, spatially confined by the tip of a single nanopipette. The exchange of matter between the two solutions determines the supersaturation, which is controlled by electrokinetic ion transport driven by an external potential waveform. Nucleation and subsequent crystal growth disrupt the ionic current limited by the nanotip and are detected. The nucleation and growth of individual single crystals are measured in real time. Electroanalytical and optical signatures are elucidated as feedbacks with which active controls in crystal quality and method consistency are achieved: five out of five crystals diffract at a true atomic resolution of up to 1.2 Å. As controls, those synthesized under less optimized conditions diffract poorly. The crystal habits during the growth process are tuned successfully by adjusting the flux. The universal mechanism of nano-transport kinetics, together with the correlations of the diffraction quality and crystal habit with the crystallization control parameters, lay the foundation for the generalization to other materials systems.
MeSH term(s)	Proteins/chemistry ; Crystallization/methods ; Phase Transition ; Kinetics
Chemical Substances	Proteins
Language	English
Publishing date	2023-05-27
Publishing country	United States
Document type	Journal Article ; Research Support, U.S. Gov't, Non-P.H.S.
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.3c00175
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Deconvolution of electroosmotic flow in hysteresis ion transport through single asymmetric nanopipettes.

Brown, Warren / Li, Yan / Yang, Ruoyu / Wang, Dengchao / Kvetny, Maksim / Zheng, Hui / Wang, Gangli

Chemical science

2020 Volume 11, Issue 23, Page(s) 5950–5958

Abstract: Unveiling the contributions of electroosmotic flow (EOF) in the electrokinetic transport through structurally-defined nanoscale pores and channels is challenging but fundamentally significant because of the broad relevance of charge transport in energy ... ...

Abstract	Unveiling the contributions of electroosmotic flow (EOF) in the electrokinetic transport through structurally-defined nanoscale pores and channels is challenging but fundamentally significant because of the broad relevance of charge transport in energy conversion, desalination and analyte mixing, micro and nano-fluidics, single entity analysis, capillary electrophoresis
Language	English
Publishing date	2020-05-19
Publishing country	England
Document type	Journal Article
ZDB-ID	2559110-1
ISSN	2041-6539 ; 2041-6520
ISSN (online)	2041-6539
ISSN	2041-6520
DOI	10.1039/c9sc06386b
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Correlation of Ion Transport Hysteresis with the Nanogeometry and Surface Factors in Single Conical Nanopores

Wang, Dengchao / Brown Warren / Kvetny Maksim / Li Yan / Liu Juan / Wang Gangli

Analytical chemistry. 2017 Nov. 07, v. 89, no. 21

2017

Abstract: Better understanding in the dynamics of ion transport through nanopores or nanochannels is important for sensing, nucleic acid sequencing and energy technology. In this paper, the intriguing nonzero cross point, resolved from the pinched hysteresis ... ...

Abstract	Better understanding in the dynamics of ion transport through nanopores or nanochannels is important for sensing, nucleic acid sequencing and energy technology. In this paper, the intriguing nonzero cross point, resolved from the pinched hysteresis currentâpotential (iâV) curves in conical nanopore electrokinetic measurements, is quantitatively correlated to the surface and geometric properties by simulation studies. The analytical descriptions of the conductance and potential at the cross point are developed: the cross-point conductance includes both the surface and volumetric conductance; the cross-point potential represent the overall/averaged surface potential difference across the nanopore. The impacts by individual parameter such as pore radius, half cone angle, and surface charges are systematically studied in the simulation that would be convoluted and challenging in experiments. The elucidated correlation is supported by and offer predictive guidance for experimental studies. The results also offer more quantitative and systematic insights in the physical origins of the concentration polarization dynamics in addition to ionic current rectification inside conical nanopores and other asymmetric nanostructures. Overall, the cross point serves as a simple yet informative analytical parameter to analyze the electrokinetic transport through broadly defined nanopore-type devices.
Keywords	energy ; geometry ; hysteresis ; ions ; nanopores
Language	English
Dates of publication	2017-1107
Size	p. 11811-11817.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021%2Facs.analchem.7b03477
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Correlation of Ion Transport Hysteresis with the Nanogeometry and Surface Factors in Single Conical Nanopores.

Wang, Dengchao / Brown, Warren / Li, Yan / Kvetny, Maksim / Liu, Juan / Wang, Gangli

Analytical chemistry

2017 Volume 89, Issue 21, Page(s) 11811–11817

Abstract	Better understanding in the dynamics of ion transport through nanopores or nanochannels is important for sensing, nucleic acid sequencing and energy technology. In this paper, the intriguing nonzero cross point, resolved from the pinched hysteresis current-potential (i-V) curves in conical nanopore electrokinetic measurements, is quantitatively correlated to the surface and geometric properties by simulation studies. The analytical descriptions of the conductance and potential at the cross point are developed: the cross-point conductance includes both the surface and volumetric conductance; the cross-point potential represent the overall/averaged surface potential difference across the nanopore. The impacts by individual parameter such as pore radius, half cone angle, and surface charges are systematically studied in the simulation that would be convoluted and challenging in experiments. The elucidated correlation is supported by and offer predictive guidance for experimental studies. The results also offer more quantitative and systematic insights in the physical origins of the concentration polarization dynamics in addition to ionic current rectification inside conical nanopores and other asymmetric nanostructures. Overall, the cross point serves as a simple yet informative analytical parameter to analyze the electrokinetic transport through broadly defined nanopore-type devices.
Language	English
Publishing date	2017-10-18
Publishing country	United States
Document type	Journal Article ; Research Support, U.S. Gov't, Non-P.H.S.
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.7b03477
Database	MEDical Literature Analysis and Retrieval System OnLINE

In stock of ZB MED Cologne/Königswinter

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Location:
Je nach Verfügbarkeit (siehe Angabe bei Bestand)
bis Jg. 1994: Bestellungen von Artikeln über das Online-Bestellformular
Jg. 1995 - 2021: Lesesall (2.OG)
ab Jg. 2022: Lesesaal (EG)

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Article: Quantification of Steady-State Ion Transport through Single Conical Nanopores and a Nonuniform Distribution of Surface Charges

Liu, Juan / Brown Warren / Kvetny Maksim / Li Yan / Wang Dengchao / Wang Gangli

Langmuir. 2013 July 09, v. 29, no. 27

2013

Abstract: Electrostatic interactions of mobile charges in solution with the fixed surface charges are known to strongly affect stochastic sensing and electrochemical energy conversion processes at nanodevices or devices with nanostructured interfaces. The key ... ...

Abstract	Electrostatic interactions of mobile charges in solution with the fixed surface charges are known to strongly affect stochastic sensing and electrochemical energy conversion processes at nanodevices or devices with nanostructured interfaces. The key parameter to describe this interaction, surface charge density (SCD), is not directly accessible at nanometer scale and often extrapolated from ensemble values. In this report, the steady-state currentâvoltage (iâV) curves measured using single conical glass nanopores in different electrolyte solutions are fitted by solving Poisson and NernstâPlanck equations through finite element approach. Both high and low conductivity state currents of the rectified iâV curve are quantitatively fitted in simulation at less than 5% error. The overestimation of low conductivity state current using existing models is overcome by the introduction of an exponential SCD distribution inside the conical nanopore. A maximum SCD value at the pore orifice is determined from the fitting of the high conductivity state current, while the distribution length of the exponential SCD gradient is determined by fitting the low conductivity state current. Quantitative fitting of the rectified iâV responses and the efficacy of the proposed model are further validated by the comparison of electrolytes with different types of cations (Kâº and Liâº). The gradient distribution of surface charges is proposed to be dependent on the local electric field distribution inside the conical nanopore.
Keywords	cations ; electric field ; electrochemistry ; electrostatic interactions ; energy conversion ; equations ; finite element analysis ; glass ; lithium ; models ; nanopores ; potassium
Language	English
Dates of publication	2013-0709
Size	p. 8743-8752.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	2005937-1
ISSN	1520-5827 ; 0743-7463
ISSN (online)	1520-5827
ISSN	0743-7463
DOI	10.1021%2Fla4009009
Database	NAL-Catalogue (AGRICOLA)

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Article: History-dependent ion transport through conical nanopipettes and the implications in energy conversion dynamics at nanoscale interfaces.

Li, Yan / Wang, Dengchao / Kvetny, Maksim M / Brown, Warren / Liu, Juan / Wang, Gangli

Chemical science

2014 Volume 6, Issue 1, Page(s) 588–595

Abstract: The dynamics of ion transport at nanostructured substrate-solution interfaces play vital roles in high-density energy conversion, stochastic chemical sensing and biosensing, membrane separation, nanofluidics and fundamental nanoelectrochemistry. Further ... ...

Abstract	The dynamics of ion transport at nanostructured substrate-solution interfaces play vital roles in high-density energy conversion, stochastic chemical sensing and biosensing, membrane separation, nanofluidics and fundamental nanoelectrochemistry. Further advancements in these applications require a fundamental understanding of ion transport at nanoscale interfaces. The understanding of the dynamic or transient transport, and the key physical process involved, is limited, which contrasts sharply with widely studied steady-state ion transport features at atomic and nanometer scale interfaces. Here we report striking time-dependent ion transport characteristics at nanoscale interfaces in current-potential (
Language	English
Publishing date	2014-08-20
Publishing country	England
Document type	Journal Article
ZDB-ID	2559110-1
ISSN	2041-6539 ; 2041-6520
ISSN (online)	2041-6539
ISSN	2041-6520
DOI	10.1039/c4sc02195a
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Surface Charge Density Determination of Single Conical Nanopores Based on Normalized Ion Current Rectification

Liu, Juan / Brown Warren / Feng Jingyu / Kvetny Maksim / Wang Dengchao / Wang Gangli / Wu Baohua

Langmuir. 2012 Jan. 17, v. 28, no. 2

2012

Abstract: Current rectification is well known in ion transport through nanoscale pores and channel devices. The measured current is affected by both the geometry and fixed interfacial charges of the nanodevices. In this article, an interesting trend is observed in ...

Abstract	Current rectification is well known in ion transport through nanoscale pores and channel devices. The measured current is affected by both the geometry and fixed interfacial charges of the nanodevices. In this article, an interesting trend is observed in steady-state currentâpotential measurements using single conical nanopores. A threshold low-conductivity state is observed upon the dilution of electrolyte concentration. Correspondingly, the normalized current at positive bias potentials drastically increases and contributes to different degrees of rectification. This novel trend at opposite bias polarities is employed to differentiate the ion flux affected by the fixed charges at the substrateâsolution interface (surface effect), with respect to the constant asymmetric geometry (volume effect). The surface charge density (SCD) of individual nanopores, an important physical parameter that is challenging to measure experimentally and is known to vary from one nanopore to another, is directly quantified by solving Poisson and NernstâPlanck equations in the simulation of the experimental results. The flux distribution inside the nanopore and the SCD of individual nanopores are reported. The respective diffusion and migration translocations are found to vary at different positions inside the nanopore. This knowledge is believed to be important for resistive pulse sensing applications because the detection signal is determined by the perturbation of the ion current by the analytes.
Keywords	electrolytes ; equations ; nanopores
Language	English
Dates of publication	2012-0117
Size	p. 1588-1595.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	2005937-1
ISSN	1520-5827 ; 0743-7463
ISSN (online)	1520-5827
ISSN	0743-7463
DOI	10.1021%2Fla203106w
Database	NAL-Catalogue (AGRICOLA)

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Article: Transmembrane Potential across Single Conical Nanopores and Resulting Memristive and Memcapacitive Ion Transport

Wang, Dengchao / Brown Warren / Kvetny Maksim / Li Yan / Liu Juan / Wang Gangli

Journal of the American Chemical Society. 2012 Feb. 29, v. 134, no. 8

2012

Abstract: Memristive and memcapacitive behaviors are observed from ion transport through single conical nanopores in SiOâ substrate. In iâV measurements, current is found to depend on not just the applied bias potential but also previous conditions in the ... ...

Abstract	Memristive and memcapacitive behaviors are observed from ion transport through single conical nanopores in SiOâ substrate. In iâV measurements, current is found to depend on not just the applied bias potential but also previous conditions in the transport-limiting region inside the nanopore (history-dependent, or memory effect). At different scan rates, a constant cross-point potential separates normal and negative hysteresis loops at low and high conductivity states, respectively. Memory effects are attributed to the finite mobility of ions as they redistribute within the negatively charged nanopore under applied potentials. A quantative correlation between the cross-point potential and electrolyte concentration is established.
Keywords	electrolytes ; hysteresis ; ions ; membrane potential ; nanopores ; silica
Language	English
Dates of publication	2012-0229
Size	p. 3651-3654.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021%2Fja211142e
Database	NAL-Catalogue (AGRICOLA)

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