Active Sulfur Sites in Semimetallic Titanium Disulfide Enable CO2 Electroreduction

被引：24

作者：

Allabour, Abdalaziz ^{[1
]}

Coskun, Halime ^{[1
]}

Zheng, Xueli ^{[5
,6
]}

Kibria, Md Golam ^{[5
,7
]}

Strobel, Moritz ^{[2
]}

Hild, Sabine ^{[2
]}

Kehrer, Matthias ^{[3
]}

Stifter, David ^{[3
]}

Sargent, Edward H. ^{[5
]}

Stadler, Philipp ^{[1
,4
,5
]}

机构：

[1] Johannes Kepler Univ Linz, Inst Phys Chem, Altenbergerstr 69, A-4040 Linz, Austria

[2] Johannes Kepler Univ Linz, Inst Polymer Sci, Altenbergerstr 69, A-4040 Linz, Austria

[3] Johannes Kepler Univ Linz, Ctr Surface & Nanoanalyt, Altenbergerstr 69, A-4040 Linz, Austria

[4] Johannes Kepler Univ Linz, Linz Inst Technol, Altenbergerstr 69, A-4040 Linz, Austria

[5] Univ Toronto, Edward S Rogers Sr Dept Elect & Comp Engn, 10 Kings Coll Rd, Toronto, ON M5S 3G4, Canada

[6] Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA

[7] Univ Calgary, Dept Chem & Petr Engn, 2500 Univ Dr NW, Calgary, AB T2N 1N4, Canada

来源：

ACS CATALYSIS | 2020年 / 10卷 / 01期

关键词：

CO2 reduction reaction; titanium disulfide; electrocatalysis; ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; FORMIC-ACID; BASAL-PLANE; SELECTIVITY; NANOSHEETS; TIS2; VACANCIES; MOS2; GAS;

D O I：

10.1021/acscatal.9b02872

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Electrocatalytic CO2-to-CO conversion represents one pathway to upgrade CO2 to a feedstock for both fuels and chemicals (CO, deployed in ensuing Fischer-Tropsch or bioupgrading). It necessitates selective and energy-efficient electrocatalysts-a requirement met today only using noble metals such as gold and silver. Here, we show that the two-dimensional sulfur planes in semimetallic titanium disulfide (TiS2) provide an earth-abundant alternative. In situ Fourier transform infrared mechanistic studies reveal that CO2 binds to conductive disulfide planes as intermediate monothiocarbonate. The sulfur-CO2 intermediate state steers the reduction kinetics toward mainly CO. Using TiS2 thin films, we reach cathodic energy efficiencies up to 64% at 5 mA cm(2). We conclude with directions for the further synthesis and study of semimetallic disulfides developing CO-selective electrocatalysts.

引用

页码：66 / 72

页数：13

共 54 条

[1] Tailoring the Edge Structure of Molybdenum Disulfide toward Electrocatalytic Reduction of Carbon Dioxide [J].

Abbasi, Pedram ;

Asadi, Mohammad ;

Liu, Cong ;

Sharifi-Asl, Soroosh ;

Sayahpour, Baharak ;

Behranginia, Amirhossein ;

Zapol, Peter ;

Shahbazian-Yassar, Reza ;

Curtiss, Larry A. ;

Salehi-Khojin, Amin .

ACS NANO, 2017, 11 (01) :453-460

[2] Heterogeneous uptake and reactivity of formic acid on calcium carbonate particles: a Knudsen cell reactor, FTIR and SEM study [J].

Al-Hosney, HA ;

Carlos-Cuellar, S ;

Baltrusaitis, J ;

Grassian, VH .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2005, 7 (20) :3587-3595

[3] IR spectra of protonated carbonic acid and its isomeric H3O+•CO2 complex [J].

Andrei, Horia-Sorin ;

Nizkorodov, Sergey A. ;

Dopfer, Otto .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (25) :4754-4756

[4] Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid [J].

Asadi, Mohammad ;

Kim, Kibum ;

Liu, Cong ;

Addepalli, Aditya Venkata ;

Abbasi, Pedram ;

Yasaei, Poya ;

Phillips, Patrick ;

Behranginia, Amirhossein ;

Cerrato, Jose M. ;

Haasch, Richard ;

Zapol, Peter ;

Kumar, Bijandra ;

Klie, Robert F. ;

Abiade, Jeremiah ;

Curtiss, Larry A. ;

Salehi-Khojin, Amin .

SCIENCE, 2016, 353 (6298) :467-470

[5] Robust carbon dioxide reduction on molybdenum disulphide edges [J].

Asadi, Mohammad ;

Kumar, Bijandra ;

Behranginia, Amirhossein ;

Rosen, Brian A. ;

Baskin, Artem ;

Repnin, Nikita ;

Pisasale, Davide ;

Phillips, Patrick ;

Zhu, Wei ;

Haasch, Richard ;

Klie, Robert F. ;

Kral, Petr ;

Abiade, Jeremiah ;

Salehi-Khojin, Amin .

NATURE COMMUNICATIONS, 2014, 5

[6] Two Dimensional TiS2 as a Promising Insertion Anode for Na-Ion Battery [J].

Chaturvedi, Apoorva ;

Edison, Eldho ;

Arun, Nagasubramanian ;

Hu, Peng ;

Kloc, Christian ;

Aravindan, Vanchiappan ;

Madhavi, Srinivasan .

CHEMISTRYSELECT, 2018, 3 (02) :524-528

[7]

Chhowalla M, 2013, NAT CHEM, V5, P263, DOI [10.1038/NCHEM.1589, 10.1038/nchem.1589]

[8] The path towards sustainable energy [J].

Chu, Steven ;

Cui, Yi ;

Liu, Nian .

NATURE MATERIALS, 2017, 16 (01) :16-22

[9] ELECTRICAL PROPERTIES OF GROUP 4 DISULFIDES TIS2 ZRS2 HFS2 AND SNS2 [J].

CONROY, L ;

PARK, KC .

INORGANIC CHEMISTRY, 1968, 7 (03) :459-&

[10] Biofunctionalized conductive polymers enable efficient CO2 electroreduction [J].

Coskun, Halime ;

Aljabour, Abdalaziz ;

De Luna, Phil ;

Farka, Dominik ;

Greunz, Theresia ;

Stifter, David ;

Kus, Mahmut ;

Zheng, Xueli ;

Liu, Min ;

Hassel, Achim W. ;

Schofberger, Wolfgang ;

Sargent, Edward H. ;

Sariciftci, Niyazi Serdar ;

Stadler, Philipp .

SCIENCE ADVANCES, 2017, 3 (08)

← 1 2 3 4 5 6 →