
当研究室では、環境調和型溶媒である「水」「CO2」「イオン液体」を研究の中心に据え、バイオマス資源の有用物質への変換や廃棄資源の再利用化プロセスの検討を行っています。また、化学工学的な視点から、プロセスの高効率化に向けた基礎物性の測定やモデル化などにも取り組んでいます。
主な研究
2019年

H. Li, H. Guo, Y. Su, Y. Hiraga, Z. Fang, E.J.M. Hensen, M. Watanabe, R.L. Smith, N-formyl-stabilizing quasi-catalytic species afford rapid and selective solvent-free amination of biomass-derived feedstocks, Nature Communications, 10 (2019).
OPEN ACCESS http://dx.doi.org/10.1038/s41467-019-08577-4
Blog in Nature Chemistry (Channels – Behind the paper) https://chemistrycommunity.nature.com/users/207387-richard-smith/posts/44026-n-formyl-stabilizing-quasi-catalytic-species
Announcement (日本語) http://www.che.tohoku.ac.jp/news/research/article.html?news_id=166

H. Guo, Y. Hiraga, X. Qi, R.L. Smith, Hydrogen gas-free processes for single-step preparation of transition-metal bifunctional catalysts and one-pot gamma-valerolactone synthesis in supercritical CO 2 -ionic liquid systems, Journal of Supercritical Fluids, 147 (2019) 263-270. http://dx.doi.org/10.1016/j.supflu.2018.11.010

T. Shida, Y. Hiraga, T. Sugiyama, Y. Sato, M. Watanabe, R.L. Smith, Measurement and modeling of infinite dilution activity coefficients of organic compounds in an equimolar ionic liquid mixture of [Bmim]Cl and [Bmim][Tf2N], Fluid Phase Equilibria, 488 (2019) 72-78.
http://dx.doi.org/10.1016/j.fluid.2019.01.028

S. Sato, M. Ota, Y. Sato, R.L. Smith, H. Inomata, Measurement and correlation
of vapor-liquid distribution coefficients of flavonoids in high pressure
carbon dioxide – ethanol – water systems, Fluid Phase Equilibria, 489 (2019)
90-98.
http://dx.doi.org/10.1016/j.fluid.2019.02.015

H. Li, Y. Li, Z. Fang, R.L. Smith, Efficient catalytic transfer hydrogenation
of biomass-based furfural to furfuryl alcohol with recycable Hf-phenylphosphonate
nanohybrids, Catalysis Today, 319 (2019) 84-92.
http://dx.doi.org/10.1016/j.cattod.2018.04.056

H. Komatsu, T. Sasagawa, S. Yamamoto, Y. Hiraga, M. Ota, T. Tsukada, R.L. Smith, Methane clathrate hydrate dissociation analyzed with Raman spectroscopy and a thermodynamic mass transfer model considering cage occupancy, Fluid Phase Equilibria, 489 (2019) 41-47.http://dx.doi.org/10.1016/j.fluid.2019.02.004
2015-2018年

H. Li, R.L. Smith, Solvents take control, Nature Catalysis, 1 (2018) 176-177.
http://dx.doi.org/10.1038/s41929-018-0040-6

E. Kiran, G. Brunner, R.L. Smith, M.J.A. Cocero, A. Welch, Preface The
30thYear Special issue of the Journal of Supercritical Fluids- Perspectives
and Opinions on Current State and Future Directions, Journal of Supercritical
Fluids, 134 (2018) 1.
http://dx.doi.org/10.1016/j.supflu.2018.02.003

A. Duereh, R.L. Smith, Strategies for using hydrogen-bond donor/acceptor
solvent pairs in developing green chemical processes with supercritical
fluids, Journal of Supercritical Fluids, 141 (2018) 182-197.
http://dx.doi.org/10.1016/j.supflu.2017.11.004

M. Watanabe, Y. Kanaguri, R.L. Smith, Hydrothermal separation of lignin
from bark of Japanese cedar, Journal of Supercritical Fluids, 133 (2018)
696-703.
http://dx.doi.org/10.1016/j.supflu.2017.09.009

F. Shen, Y. Wang, L. Li, K. Zhang, R.L. Smith, X. Qi, Porous carbonaceous materials from hydrothermal carbonization and KOH activation of corn stover for highly efficient CO2 capture, Chemical Engineering Communications, 205 (2018) 423-431. http://dx.doi.org/10.1080/00986445.2017.1367671

T. Sato, T. Takahata, T. Honma, M. Watanabe, M. Wagatsuma, S. Matsuda,
R.L. Smith, N. Itoh, Hydrothermal Extraction of Antioxidant Compounds from
Green Coffee Beans and Decomposition Kinetics of 3- o-Caffeoylquinic Acid,
Industrial and Engineering Chemistry Research, 57 (2018) 7624-7632.
http://dx.doi.org/10.1021/acs.iecr.8b00821

M. Ota, Y. Sato, R.L. Smith, H. Inomata, Predictive dimensionless solubility
(pDS) model for solid solutes in supercritical CO2 that requires only pure-component
physical properties, Chemical Engineering Research and Design, 136 (2018)
251-261.
http://dx.doi.org/10.1016/j.cherd.2018.04.033

W.J. Lee, C.P. Tan, R. Sulaiman, R.L. Smith, G.H. Chong, Microencapsulation
of red palm oil as an oil-in-water emulsion with supercritical carbon dioxide
solution-enhanced dispersion, Journal of Food Engineering, 222 (2018) 100-109.
http://dx.doi.org/10.1016/j.jfoodeng.2017.11.011

Y. Hoshino, M. Ota, Y. Sato, R.L. Smith, H. Inomata, Fractionation of hops-extract–ethanol
solutions using dense CO2 with a counter-current extraction column, Journal
of Supercritical Fluids, 136 (2018) 37-43.
http://dx.doi.org/10.1016/j.supflu.2018.02.005

Y. Hiraga, K. Koyama, Y. Sato, R.L. Smith, Measurement and modeling of
CO2 solubility in [bmim]Cl – [bmim][Tf2N] mixed-ionic liquids for design
of versatile reaction solvents, Journal of Supercritical Fluids, 132 (2018)
42-50.
http://dx.doi.org/10.1016/j.supflu.2017.02.001

Y. Hiraga, S. Hagiwara, Y. Sato, R.L. Smith, Measurement and Correlation
of High-Pressure Densities and Atmospheric Viscosities of Ionic Liquids:
1-Butyl-1-methylpyrrolidinium Bis(trifluoromethylsulfonyl)imide), 1-Allyl-3-methylimidazolium
Bis(trifluoromethylsulfonyl)imide, 1-Ethyl-3-methylimidazolium Tetracyanoborate,
and 1-Hexyl-3-methylimidazolium Tetracyanoborate, Journal of Chemical and
Engineering Data, 63 (2018) 972-980.
http://dx.doi.org/10.1021/acs.jced.7b00773

Y. Hiraga, A. Duereh, R.L. Smith, Aspects of solvent polarity and solvent
properties in developing efficient systems for processing biomass with
ionic liquid mixtures and supercritical CO2, Journal of Supercritical Fluids,
134 (2018) 12-20.
http://dx.doi.org/10.1016/j.supflu.2017.12.022

H. Guo, A. Duereh, Y. Hiraga, X. Qi, R.L. Smith, Mechanism of Glucose Conversion
into 5-Ethoxymethylfurfural in Ethanol with Hydrogen Sulfate Ionic Liquid
Additives and a Lewis Acid Catalyst, Energy and Fuels, 32 (2018) 8411-8419.
http://dx.doi.org/10.1021/acs.energyfuels.8b00717

A. Duereh, Y. Sato, R.L. Smith, H. Inomata, Correspondence between Spectral-Derived and Viscosity-Derived Local Composition in Binary Liquid Mixtures Having Specific Interactions with Preferential Solvation Theory, Journal of Physical Chemistry B, 122 (2018) 10894-10906. http://dx.doi.org/10.1021/acs.jpcb.8b09511

A. Duereh, H. Guo, T. Honma, Y. Hiraga, Y. Sato, R. Lee Smith, H. Inomata,
Solvent Polarity of Cyclic Ketone (Cyclopentanone, Cyclohexanone): Alcohol
(Methanol, Ethanol) Renewable Mixed-Solvent Systems for Applications in
Pharmaceutical and Chemical Processing, Industrial and Engineering Chemistry
Research, 57 (2018) 7331-7344.
http://dx.doi.org/10.1021/acs.iecr.8b00689

L. Zhu, F. Shen, R.L. Smith, L. Yan, L. Li, X. Qi, Black liquor-derived
porous carbons from rice straw for high-performance supercapacitors, Chemical
Engineering Journal, 316 (2017) 770-777.
http://dx.doi.org/10.1016/j.cej.2017.02.034

L. Zhu, F. Shen, R.L. Smith, X. Qi, High-Performance Supercapacitor Electrode
Materials from Chitosan via Hydrothermal Carbonization and Potassium Hydroxide
Activation, Energy Technology, 5 (2017) 452-460.
http://dx.doi.org/10.1002/ente.201600337

I. Ushiki, M. Tashiro, R.L. Smith, Measurement and modeling of adsorption
equilibria of imidazolium-based ionic liquids on activated carbon from
aqueous solutions, Fluid Phase Equilibria, 441 (2017) 17-23.
http://dx.doi.org/10.1016/j.fluid.2017.01.021

I. Ushiki, N. Takahashi, T. Shimizu, Y. Sato, M. Ota, R.L. Smith, H. Inomata,
Adsorption equilibria of rhodium acetylacetonate with MCM-41, MSU-H, and
HMS silica substrates in supercritical carbon dioxide for preparing catalytic
mesoporous materials, Journal of Supercritical Fluids, 120 (2017) 240-248.
http://dx.doi.org/10.1016/j.supflu.2016.05.032

F. Shen, R.L. Smith, L. Li, L. Yan, X. Qi, Eco-friendly Method for Efficient
Conversion of Cellulose into Levulinic Acid in Pure Water with Cellulase-Mimetic
Solid Acid Catalyst, ACS Sustainable Chemistry and Engineering, 5 (2017)
2421-2427.
http://dx.doi.org/10.1021/acssuschemeng.6b02765

M. Ota, S. Sugahara, Y. Sato, R.L. Smith, H. Inomata, Vapor-liquid distribution coefficients of hops extract in high pressure CO2 and ethanol mixtures and data correlation with entropy-based solubility parameters, Fluid Phase Equilibria, 434 (2017) 44-48.http://dx.doi.org/10.1016/j.fluid.2016.11.011

M. Ota, M. Sato, Y. Sato, R.L. Smith, H. Inomata, Measurement and correlation
of flavanone, tangeritin, nobiletin, 6-hydroxyflavanone and 7-hydroxyflavone
solubilities in supercritical CO2, Journal of Supercritical Fluids, 128
(2017) 166-172.
http://dx.doi.org/10.1016/j.supflu.2017.05.024

K. Okada, H. Hayashi, M. Takesue, M. Watanabe, R.L. Smith, Synthesis of
ferroelectric K1-xNaxNb1-yTayO3 nanoparticles using a supercritical water
flow system, Journal of Supercritical Fluids, 123 (2017) 101-108.
http://dx.doi.org/10.1016/j.supflu.2016.12.018

L. Li, F. Shen, R.L. Smith, X. Qi, Quantitative chemocatalytic production
of lactic acid from glucose under anaerobic conditions at room temperature,
Green Chemistry, 19 (2017) 76-81.
http://dx.doi.org/10.1039/c6gc02443b

Y. Hiraga, M. Goto, Y. Sato, R.L. Smith, Measurement of high pressure densities and atmospheric pressure viscosities of alkyl phosphate anion ionic liquids and correlation with the ε∗-modified Sanchez-Lacombe equation of state, Journal of Chemical Thermodynamics, 104 (2017) 73-81. http://dx.doi.org/10.1016/j.jct.2016.09.013

Y.Y. Hee, C.P. Tan, R.A. Rahman, M. Noranizan, R.L. Smith, G.H. Chong,
Production of virgin coconut oil microcapsules from oil-in-water emulsion
with supercritical carbon dioxide spray drying, Journal of Supercritical
Fluids, 130 (2017) 118-124.
http://dx.doi.org/10.1016/j.supflu.2017.07.037

H. Guo, X. Qi, Y. Hiraga, T.M. Aida, R.L. Smith, Efficient conversion of
fructose into 5-ethoxymethylfurfural with hydrogen sulfate ionic liquids
as co-solvent and catalyst, Chemical Engineering Journal, 314 (2017) 508-514.
http://dx.doi.org/10.1016/j.cej.2016.12.008

H. Guo, A. Duereh, Y. Hiraga, T.M. Aida, X. Qi, R.L. Smith, Perfect recycle and mechanistic role of hydrogen sulfate ionic liquids as additive in ethanol for efficient conversion of carbohydrates into 5-ethoxymethylfurfural, Chemical Engineering Journal, 323 (2017) 287-294. http://dx.doi.org/10.1016/j.cej.2017.04.111

A. Duereh, Y. Sato, R.L. Smith, H. Inomata, F. Pichierri, Does Synergism in Microscopic Polarity Correlate with Extrema in Macroscopic Properties for Aqueous Mixtures of Dipolar Aprotic Solvents?, Journal of Physical Chemistry B, 121 (2017) 6033-6041. http://dx.doi.org/10.1021/acs.jpcb.7b03446

A. Duereh, Y. Sato, R.L. Smith, H. Inomata, Methodology for replacing dipolar
aprotic solvents used in API processing with safe hydrogen-bond donor and
acceptor solvent-pair mixtures, Organic Process Research and Development,
21 (2017) 114-124. OPEN ACCESS http://dx.doi.org/10.1021/acs.oprd.6b00401
Safe Solvent-Pair Mixtures Software (Microsoft Excel – Zip File)
https://pubs.acs.org/doi/suppl/10.1021/acs.oprd.6b00401/suppl_file/op6b00401_si_002.zip

T.M. Aida, M. Oshima, R.L. Smith, Controlled Conversion of Proteins into High-Molecular-Weight Peptides without Additives with High-Temperature Water and Fast Heating Rates, ACS Sustainable Chemistry and Engineering, 5 (2017) 7709-7715. http://dx.doi.org/10.1021/acssuschemeng.7b01146

T.M. Aida, R. Maruta, Y. Tanabe, M. Oshima, T. Nonaka, H. Kujiraoka, Y.
Kumagai, M. Ota, I. Suzuki, M.M. Watanabe, H. Inomata, R.L. Smith, Nutrient
recycle from defatted microalgae (Aurantiochytrium) with hydrothermal treatment
for microalgae cultivation, Bioresource Technology, 228 (2017) 186-192.
http://dx.doi.org/10.1016/j.biortech.2016.12.078

H. Zhong, M. Watanabe, H. Enomoto, F. Jin, A. Kishita, T.M. Aida, R.L. Smith, Winterization of Vegetable Oil Blends for Biodiesel Fuels and Correlation Based on Initial Saturated Fatty Acid Constituents, Energy and Fuels, 30 (2016) 4841-4847. http://dx.doi.org/10.1021/acs.energyfuels.6b00310

S. Toyama, H. Hayashi, M. Takesue, M. Watanabe, R.L. Smith, Synthesis of
alkali niobate K1-xNaxNbO3 nanoparticles using a supercritical water flow
system, Journal of Supercritical Fluids, 107 (2016) 1-8.
http://dx.doi.org/10.1016/j.supflu.2015.08.008

M. Ota, Y. Hashimoto, M. Sato, Y. Sato, R.L. Smith, H. Inomata, Solubility
of flavone, 6-methoxyflavone and anthracene in supercritical CO2 with/without
a co-solvent of ethanol correlated by using a newly proposed entropy-based
solubility parameter, Fluid Phase Equilibria, 425 (2016) 65-71.
http://dx.doi.org/10.1016/j.fluid.2016.05.009

T. Morioka, M. Takesue, H. Hayashi, M. Watanabe, R.L. Smith, Antioxidation Properties and Surface Interactions of Polyvinylpyrrolidone-Capped Zerovalent Copper Nanoparticles Synthesized in Supercritical Water, ACS Applied Materials and Interfaces, 8 (2016) 1627-1634. http://dx.doi.org/10.1021/acsami.5b07566

H. Li, Z. Fang, R.L. Smith, S. Yang, Efficient valorization of biomass
to biofuels with bifunctional solid catalytic materials, Progress in Energy
and Combustion Science, 55 (2016) 98-194.
http://dx.doi.org/10.1016/j.pecs.2016.04.004

H. Kitajima, Y. Higashino, S. Matsuda, H. Zhong, M. Watanabe, T.M. Aida,
R.L. Smith, Isomerization of glucose at hydrothermal condition with TiO2,
ZrO2, CaO-doped ZrO2 or TiO2-doped ZrO2, Catalysis Today, 274 (2016) 67-72.
http://dx.doi.org/10.1016/j.cattod.2016.01.049

Y. Hiraga, Y. Sato, R.L. Smith, Measurement of infinite dilution partition
coefficients of isomeric benzene derivatives in [bmim][Tf2N]-CO2 biphasic
system and correlation with the ePC-SAFT equation of state, Fluid Phase
Equilibria, 420 (2016) 36-43.
http://dx.doi.org/10.1016/j.fluid.2015.10.042

Y. Hiraga, A. Kato, Y. Sato, T.M. Aida, M. Watanabe, R.L. Smith, Separation
factors for [amim]Cl-CO2 biphasic systems from high pressure density and
partition coefficient measurements, Separation and Purification Technology,
155 (2016).
http://dx.doi.org/10.1016/j.seppur.2015.03.008

A. Duereh, Y. Sato, R.L. Smith, H. Inomata, Analysis of the Cybotactic
Region of Two Renewable Lactone-Water Mixed-Solvent Systems that Exhibit
Synergistic Kamlet-Taft Basicity, Journal of Physical Chemistry B, 120
(2016) 4467-4481.
http://dx.doi.org/10.1021/acs.jpcb.6b03090

T.M. Aida, T. Nonaka, S. Fukuda, H. Kujiraoka, Y. Kumagai, R. Maruta, M.
Ota, I. Suzuki, M.M. Watanabe, H. Inomata, R.L. Smith, Nutrient recovery
from municipal sludge for microalgae cultivation with two-step hydrothermal
liquefaction, Algal Research, 18 (2016) 61-68. http://dx.doi.org/10.1016/j.algal.2016.06.009

A. Duereh, Y. Sato, R.L. Smith, H. Inomata, Replacement of Hazardous Chemicals Used in Engineering Plastics with Safe and Renewable Hydrogen-Bond Donor and Acceptor Solvent-Pair Mixtures, ACS Sustainable Chemistry and Engineering, 3 (2015) 1881-1889. http://dx.doi.org/10.1021/acssuschemeng.5b00474

S. Toyama, M. Takesue, T.M. Aida, M. Watanabe, R.L. Smith, Easy emission-color-control
of Mn-doped zinc silicate phosphor by use of pH and supercritical water
conditions, Journal of Supercritical Fluids, 98 (2015) 65-69.
http://dx.doi.org/10.1016/j.supflu.2015.01.007

Y. Hiraga, Y. Sato, R.L. Smith, Development of a simple method for predicting
CO2 enhancement of H2 gas solubility in ionic liquids, Journal of Supercritical
Fluids, 96 (2015) 162-170.
http://dx.doi.org/10.1016/j.supflu.2014.09.010

Y. Hiraga, A. Kato, Y. Sato, R.L. Smith, Densities at pressures up to 200 MPa and atmospheric pressure viscosities of ionic liquids 1-ethyl-3-methylimidazolium methylphosphate, 1-ethyl-3-methylimidazolium diethylphosphate, 1-butyl-3-methylimidazolium acetate, and 1-butyl-3-methylimidazolium Bis(trifluoromethylsulfonyl)imide, Journal of Chemical and Engineering Data, 60 (2015) 876-885. http://dx.doi.org/10.1021/je5009679

A. Duereh, Y. Sato, R.L. Smith, H. Inomata, Spectroscopic Analysis of Binary Mixed-Solvent-Polyimide Precursor Systems with the Preferential Solvation Model for Determining Solute-Centric Kamlet-Taft Solvatochromic Parameters, Journal of Physical Chemistry B, 119 (2015) 14738-14749. http://dx.doi.org/10.1021/acs.jpcb.5b07751

M. Ota, M. Takenaka, Y. Sato, R.L. Smith, H. Inomata, Variation of photoautotrophic fatty acid production from a highly CO2 tolerant alga, Chlorococcum littorale, with inorganic carbon over narrow ranges of pH, Biotechnology Progress, 31 (2015) 1053-1057. http://dx.doi.org/10.1002/btpr.2099

M. Ota, M. Takenaka, Y. Sato, R. Lee Smith, H. Inomata, Effects of light
intensity and temperature on photoautotrophic growth of a green microalga,
Chlorococcum littorale, Biotechnology Reports, 7 (2015) 24-29.
http://dx.doi.org/10.1016/j.btre.2015.05.001

Y. Maeta, M. Ota, Y. Sato, R.L. Smith, H. Inomata, Measurements of vapor-liquid equilibrium in both binary carbon dioxide-ethanol and ternary carbon dioxide-ethanol-water systems with a newly developed flow-type apparatus, Fluid Phase Equilibria, 405 (2015) 96-100. http://dx.doi.org/10.1016/j.fluid.2015.07.025

H. Komatsu, M. Ota, Y. Sato, M. Watanabe, R.L. Smith, Hydrogen and carbon
dioxide adsorption with Tetra-n-Butyl ammonium semi-clathrate hydrates
for gas separations, AIChE Journal, 61 (2015) 992-1003.
http://dx.doi.org/10.1002/aic.14689

M. Iguchi, Y. Hiraga, K. Kasuya, T.M. Aida, M. Watanabe, Y. Sato, R.L. Smith, Viscosity and density of poly(ethylene glycol) and its solution with carbon dioxide at 353.2 K and 373.2 K at pressures up to 15 MPa, Journal of Supercritical Fluids, 97 (2015) 63-73. http://dx.doi.org/10.1016/j.supflu.2014.10.013