Atomistic simulations of cellulose nanofibrils and their aggregates in water

Antti Paajanen, Yogesh Sonavane, Thaddeus Maloney, Sami Paavilainen, Jukka Ketoja

Research output: Contribution to conferenceConference AbstractScientific

Abstract

The cellulose nanofibril aggregate is a fundamental hierarchical structure in many man-made cellulosic materials. Such aggregates are formed in pulp fibers, when the lignin-hemicellulose matrix is removed during chemical pulping. Further processing steps such as drying, oxidation and mechanical processing can affect the structure of these aggregates, which is reflected in the macroscopic properties of the finished product. Moreover, the interactions between the nanofibrils can be greatly affected by water penetration into the aggregate structure. We carried out a series of atomistic molecular dynamics simulations to study the aggregation and disintegration properties of cellulose nanofibrils, and the penetration of water into their aggregates. In the first study [1], we considered the interactions between carboxylated (TEMPO-oxidized) cellulose nanofibrils at various functionalization levels. The averaged interaction over multiple charge configurations reflected experimentally measured changes in the disintegration energy of TEMPO-oxidized cellulose fibers. However, the interaction strength turned out to be highly sensitive to the charge configuration. Strong deviations from the average interaction could explain the wide fibril-size distribution observed experimentally at intermediate functionalization levels. In the second study, we simulated water penetration into a compact nanofibril aggregate, with the individual fibrils separated by amorphous cellulose chains. The observed diffusion rate was comparable to that found e.g. in NMR measurements for relatively dry wood fibers. The diffusion causes rapid changes in the inter-fibril morphology, which may affect the strength and dimensional stability of structures comprised of such fibril aggregates.
Original languageEnglish
Publication statusPublished - 2017
MoE publication typeNot Eligible
Event4th International Cellulose Conference - Fukuoka, Japan
Duration: 17 Oct 201720 Oct 2017

Conference

Conference4th International Cellulose Conference
CountryJapan
CityFukuoka
Period17/10/1720/10/17

Fingerprint

cellulose
water
simulation
penetration
disintegration
interactions
fibers
dimensional stability
lignin
configurations
drying
molecular dynamics
deviation
nuclear magnetic resonance
oxidation
causes
products
matrices

Keywords

  • cellulose
  • nanofibril
  • aggregate
  • water
  • molecular dynamics
  • ProperTune

Cite this

Paajanen, A., Sonavane, Y., Maloney, T., Paavilainen, S., & Ketoja, J. (2017). Atomistic simulations of cellulose nanofibrils and their aggregates in water. Abstract from 4th International Cellulose Conference, Fukuoka, Japan.
Paajanen, Antti ; Sonavane, Yogesh ; Maloney, Thaddeus ; Paavilainen, Sami ; Ketoja, Jukka. / Atomistic simulations of cellulose nanofibrils and their aggregates in water. Abstract from 4th International Cellulose Conference, Fukuoka, Japan.
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author = "Antti Paajanen and Yogesh Sonavane and Thaddeus Maloney and Sami Paavilainen and Jukka Ketoja",
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Paajanen, A, Sonavane, Y, Maloney, T, Paavilainen, S & Ketoja, J 2017, 'Atomistic simulations of cellulose nanofibrils and their aggregates in water' 4th International Cellulose Conference, Fukuoka, Japan, 17/10/17 - 20/10/17, .

Atomistic simulations of cellulose nanofibrils and their aggregates in water. / Paajanen, Antti; Sonavane, Yogesh; Maloney, Thaddeus; Paavilainen, Sami; Ketoja, Jukka.

2017. Abstract from 4th International Cellulose Conference, Fukuoka, Japan.

Research output: Contribution to conferenceConference AbstractScientific

TY - CONF

T1 - Atomistic simulations of cellulose nanofibrils and their aggregates in water

AU - Paajanen, Antti

AU - Sonavane, Yogesh

AU - Maloney, Thaddeus

AU - Paavilainen, Sami

AU - Ketoja, Jukka

N1 - Abstracts + extended 1 page abstracts only

PY - 2017

Y1 - 2017

N2 - The cellulose nanofibril aggregate is a fundamental hierarchical structure in many man-made cellulosic materials. Such aggregates are formed in pulp fibers, when the lignin-hemicellulose matrix is removed during chemical pulping. Further processing steps such as drying, oxidation and mechanical processing can affect the structure of these aggregates, which is reflected in the macroscopic properties of the finished product. Moreover, the interactions between the nanofibrils can be greatly affected by water penetration into the aggregate structure. We carried out a series of atomistic molecular dynamics simulations to study the aggregation and disintegration properties of cellulose nanofibrils, and the penetration of water into their aggregates. In the first study [1], we considered the interactions between carboxylated (TEMPO-oxidized) cellulose nanofibrils at various functionalization levels. The averaged interaction over multiple charge configurations reflected experimentally measured changes in the disintegration energy of TEMPO-oxidized cellulose fibers. However, the interaction strength turned out to be highly sensitive to the charge configuration. Strong deviations from the average interaction could explain the wide fibril-size distribution observed experimentally at intermediate functionalization levels. In the second study, we simulated water penetration into a compact nanofibril aggregate, with the individual fibrils separated by amorphous cellulose chains. The observed diffusion rate was comparable to that found e.g. in NMR measurements for relatively dry wood fibers. The diffusion causes rapid changes in the inter-fibril morphology, which may affect the strength and dimensional stability of structures comprised of such fibril aggregates.

AB - The cellulose nanofibril aggregate is a fundamental hierarchical structure in many man-made cellulosic materials. Such aggregates are formed in pulp fibers, when the lignin-hemicellulose matrix is removed during chemical pulping. Further processing steps such as drying, oxidation and mechanical processing can affect the structure of these aggregates, which is reflected in the macroscopic properties of the finished product. Moreover, the interactions between the nanofibrils can be greatly affected by water penetration into the aggregate structure. We carried out a series of atomistic molecular dynamics simulations to study the aggregation and disintegration properties of cellulose nanofibrils, and the penetration of water into their aggregates. In the first study [1], we considered the interactions between carboxylated (TEMPO-oxidized) cellulose nanofibrils at various functionalization levels. The averaged interaction over multiple charge configurations reflected experimentally measured changes in the disintegration energy of TEMPO-oxidized cellulose fibers. However, the interaction strength turned out to be highly sensitive to the charge configuration. Strong deviations from the average interaction could explain the wide fibril-size distribution observed experimentally at intermediate functionalization levels. In the second study, we simulated water penetration into a compact nanofibril aggregate, with the individual fibrils separated by amorphous cellulose chains. The observed diffusion rate was comparable to that found e.g. in NMR measurements for relatively dry wood fibers. The diffusion causes rapid changes in the inter-fibril morphology, which may affect the strength and dimensional stability of structures comprised of such fibril aggregates.

KW - cellulose

KW - nanofibril

KW - aggregate

KW - water

KW - molecular dynamics

KW - ProperTune

M3 - Conference Abstract

ER -

Paajanen A, Sonavane Y, Maloney T, Paavilainen S, Ketoja J. Atomistic simulations of cellulose nanofibrils and their aggregates in water. 2017. Abstract from 4th International Cellulose Conference, Fukuoka, Japan.