TY - JOUR
T1 - Highly Efficient Solar-Driven Carbon Dioxide Reduction on Molybdenum Disulfide Catalyst Using Choline Chloride-Based Electrolyte
AU - Asadi, Mohammad
AU - Motevaselian, Mohammad Hossein
AU - Moradzadeh, Alireza
AU - Majidi, Leily
AU - Esmaeilirad, Mohammadreza
AU - Sun, Tao Victor
AU - Liu, Cong
AU - Bose, Rumki
AU - Abbasi, Pedram
AU - Zapol, Peter
AU - Khodadoust, Amid P.
AU - Curtiss, Larry A.
AU - Aluru, Narayana R.
AU - Salehi-Khojin, Amin
N1 - M.A. and M.H.M. contributed equally to this work. A.S.-K. R.B., P.A., and L.M.'s work was supported by the National Science Foundation (NSF, Grant #NSF-CBET-1512647 and NSF-DMREF Award #1729420). T.V.S., M.H.M, A.M., and N.R.A. were supported by the NSF under Grant Nos. 1420882, 1506619, 1545907, and 1708852. The authors acknowledge the use of the parallel computing resource Blue Waters provided by the University of Illinois and the National Center for Supercomputing Applications. C.L.'s work at Argonne National Laboratory (ANL) was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357, with UChicago Argonne, LLC, the operator of ANL. L.A.C. and P.Z.'s efforts were supported by DOE, Office of Science, BES-Materials Science and Engineering, under Contract No. DE-AC-02-06CH11357, with UChicago Argonne, LLC, the operator of ANL. M.A. and M.E.'s work were supported by Illinois Institute of Technology start-up funding, Wanger Institute for Sustainable Energy Research (WISER) seed fund (262029 221E 2300) and the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource seed funding at Northwestern University. The authors also acknowledge Dr. Rao Tatavarti from Micro-Link Device, Inc. at Chicago for providing the triple junction PV cell and Lisha Wu at the University of Illinois at Chicago for potassium (K+) analysis. A.S.-K. and M.A. conceived the idea.
M.A. and M.H.M. contributed equally to this work. A.S.-K. R.B., P.A., and L.M.’s work was supported by the National Science Foundation (NSF, Grant #NSF-CBET-1512647 and NSF-DMREF Award #1729420). T.V.S., M.H.M, A.M., and N.R.A. were supported by the NSF under Grant Nos. 1420882, 1506619, 1545907, and 1708852. The authors acknowledge the use of the parallel computing resource Blue Waters provided by the University of Illinois and the National Center for Supercomputing Applications. C.L.’s work at Argonne National Laboratory (ANL) was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC02-06CH11357, with UChicago Argonne, LLC, the operator of ANL. L.A.C. and P.Z.’s efforts were supported by DOE, Office of Science, BES-Materials Science and Engineering, under Contract No. DE-AC-02-06CH11357, with UChicago Argonne, LLC, the operator of ANL. M.A. and M.E.’s work were supported by Illinois Institute of Technology start-up funding, Wanger Institute for Sustainable Energy Research (WISER) seed fund (262029 221E 2300) and the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource seed funding at Northwestern University. The authors also acknowledge Dr. Rao Tatavarti from Micro-Link Device, Inc. at Chicago for providing the triple junction PV cell and Lisha Wu at the University of Illinois at Chicago for potassium (K+) analysis. A.S.-K. and M.A. conceived the idea. M.A. performed the flow cell and solar driven electrochemical experiments. M.A., L.M., M.E., R.B., and P.A. performed three electrode experiments and characterizations. A.S.K. supervised the electrochemical and characterization experiments. M.H.M. and A.M. performed classical MD simulations, T.V.S. performed DFT calculations, all under the supervision of N.R.A., C.L., P.Z., and L.A.C. contributed to the DFT calculation. A.K. performed flame atomic absorption spectroscopy experiments.
PY - 2019/3/6
Y1 - 2019/3/6
N2 - Conversion of CO 2 to energy-rich chemicals using renewable energy is of much interest to close the anthropogenic carbon cycle. However, the current photoelectrochemical systems are still far from being practically feasible. Here the successful demonstration of a continuous, energy efficient, and scalable solar-driven CO 2 reduction process based on earth-abundant molybdenum disulfide (MoS 2 ) catalyst, which works in synergy with an inexpensive hybrid electrolyte of choline chloride (a common food additive for livestock) and potassium hydroxide (KOH) is reported. The CO 2 saturated hybrid electrolyte utilized in this study also acts as a buffer solution (pH ≈ 7.6) to adjust pH during the reactions. This study reveals that this system can efficiently convert CO 2 to CO with solar-to-fuel and catalytic conversion efficiencies of 23% and 83%, respectively. Using density functional theory calculations, a new reaction mechanism in which the water molecules near the MoS 2 cathode act as proton donors to facilitate the CO 2 reduction process by MoS 2 catalyst is proposed. This demonstration of a continuous, cost-effective, and energy efficient solar driven CO 2 conversion process is a key step toward the industrialization of this technology.
AB - Conversion of CO 2 to energy-rich chemicals using renewable energy is of much interest to close the anthropogenic carbon cycle. However, the current photoelectrochemical systems are still far from being practically feasible. Here the successful demonstration of a continuous, energy efficient, and scalable solar-driven CO 2 reduction process based on earth-abundant molybdenum disulfide (MoS 2 ) catalyst, which works in synergy with an inexpensive hybrid electrolyte of choline chloride (a common food additive for livestock) and potassium hydroxide (KOH) is reported. The CO 2 saturated hybrid electrolyte utilized in this study also acts as a buffer solution (pH ≈ 7.6) to adjust pH during the reactions. This study reveals that this system can efficiently convert CO 2 to CO with solar-to-fuel and catalytic conversion efficiencies of 23% and 83%, respectively. Using density functional theory calculations, a new reaction mechanism in which the water molecules near the MoS 2 cathode act as proton donors to facilitate the CO 2 reduction process by MoS 2 catalyst is proposed. This demonstration of a continuous, cost-effective, and energy efficient solar driven CO 2 conversion process is a key step toward the industrialization of this technology.
KW - flow cells
KW - photochemical
KW - photoelectrochemical
KW - solar to fuel conversion
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U2 - 10.1002/aenm.201803536
DO - 10.1002/aenm.201803536
M3 - Article
AN - SCOPUS:85060348617
SN - 1614-6832
VL - 9
JO - Advanced Energy Materials
JF - Advanced Energy Materials
IS - 9
M1 - 1803536
ER -