Single Atomic Vacancy Catalysis
Single atom catalysts provide exceptional activity. However, measuring the intrinsic catalytic activity of a single atom in real electrochemical environments is challenging. Here, we report the activity of a single vacancy for electrocatalytically evolving hydrogen in two-dimensional (2D) MoS2. Surp...
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| Published in | ACS nano Vol. 13; no. 9; pp. 9958 - 9964 |
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| Main Authors | , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
24.09.2019
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| Subjects | |
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| Abstract | Single atom catalysts provide exceptional activity. However, measuring the intrinsic catalytic activity of a single atom in real electrochemical environments is challenging. Here, we report the activity of a single vacancy for electrocatalytically evolving hydrogen in two-dimensional (2D) MoS2. Surprisingly, we find that the catalytic activity per vacancy is not constant but increases with its concentration, reaching a sudden peak in activity at 5.7 × 1014 cm–2 where the intrinsic turn over frequency and Tafel slope of a single atomic vacancy was found to be ∼5 s–1 and 44 mV/dec, respectively. At this vacancy concentration, we also find a local strain of ∼3% and a semiconductor to metal transition in 2D MoS2. Our results suggest that, along with increasing the number of active sites, engineering the local strain and electrical conductivity of catalysts is essential in increasing their activity. |
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| AbstractList | Single atom catalysts provide exceptional activity. However, measuring the intrinsic catalytic activity of a single atom in real electrochemical environments is challenging. Here, we report the activity of a single vacancy for electrocatalytically evolving hydrogen in two-dimensional (2D) MoS2. Surprisingly, we find that the catalytic activity per vacancy is not constant but increases with its concentration, reaching a sudden peak in activity at 5.7 × 1014 cm–2 where the intrinsic turn over frequency and Tafel slope of a single atomic vacancy was found to be ∼5 s–1 and 44 mV/dec, respectively. At this vacancy concentration, we also find a local strain of ∼3% and a semiconductor to metal transition in 2D MoS2. Our results suggest that, along with increasing the number of active sites, engineering the local strain and electrical conductivity of catalysts is essential in increasing their activity. Single atom catalysts provide exceptional activity. However, measuring the intrinsic catalytic activity of a single atom in real electrochemical environments is challenging. Here, we report the activity of a single vacancy for electrocatalytically evolving hydrogen in two-dimensional (2D) MoS . Surprisingly, we find that the catalytic activity per vacancy is not constant but increases with its concentration, reaching a sudden peak in activity at 5.7 × 10 cm where the intrinsic turn over frequency and Tafel slope of a single atomic vacancy was found to be ∼5 s and 44 mV/dec, respectively. At this vacancy concentration, we also find a local strain of ∼3% and a semiconductor to metal transition in 2D MoS . Our results suggest that, along with increasing the number of active sites, engineering the local strain and electrical conductivity of catalysts is essential in increasing their activity. Single atom catalysts provide exceptional activity. However, measuring the intrinsic catalytic activity of a single atom in real electrochemical environments is challenging. Here, we report the activity of a single vacancy for electrocatalytically evolving hydrogen in two-dimensional (2D) MoS2. Surprisingly, we find that the catalytic activity per vacancy is not constant but increases with its concentration, reaching a sudden peak in activity at 5.7 x 10(14) cm(-2) where the intrinsic turn over frequency and Tafel slope of a single atomic vacancy was found to be similar to 5 s(-1) and 44 mV/dec, respectively. At this vacancy concentration, we also find a local strain of similar to 3% and a semiconductor to metal transition in 2D MoS2. Our results suggest that, along with increasing the number of active sites, engineering the local strain and electrical conductivity of catalysts is essential in increasing their activity. |
| Author | Yang, Jieun Manichev, Viacheslav Zhang, Wenjing Wang, Yan Chhowalla, Manish Chakraborty, Sudip Batson, Philip E Lagos, Maureen J Song, Xiuju Gustafsson, Torgny Fullon, Raymond Feldman, Leonard Voiry, Damien |
| AuthorAffiliation | Institute of Advanced Materials, Devices, and Nanotechnology McMaster University Materials Science and Engineering International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology Institut Europeen des Membranes Materials Science and Metallurgy Department of Physics and Astronomy Rutgers University Indian Institute of Technology (IIT) Indore Department of Materials Science and Engineering Department of Chemistry and Chemical Biology Discipline of Physics |
| AuthorAffiliation_xml | – name: McMaster University – name: Discipline of Physics – name: Department of Chemistry and Chemical Biology – name: Indian Institute of Technology (IIT) Indore – name: Department of Physics and Astronomy – name: Institut Europeen des Membranes – name: International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology – name: Materials Science and Metallurgy – name: Rutgers University – name: Materials Science and Engineering – name: Institute of Advanced Materials, Devices, and Nanotechnology – name: Department of Materials Science and Engineering |
| Author_xml | – sequence: 1 givenname: Jieun orcidid: 0000-0001-7053-388X surname: Yang fullname: Yang, Jieun organization: Materials Science and Metallurgy – sequence: 2 givenname: Yan surname: Wang fullname: Wang, Yan organization: Materials Science and Metallurgy – sequence: 3 givenname: Maureen J surname: Lagos fullname: Lagos, Maureen J organization: McMaster University – sequence: 4 givenname: Viacheslav surname: Manichev fullname: Manichev, Viacheslav organization: Department of Physics and Astronomy – sequence: 5 givenname: Raymond surname: Fullon fullname: Fullon, Raymond organization: Rutgers University – sequence: 6 givenname: Xiuju orcidid: 0000-0001-9777-7016 surname: Song fullname: Song, Xiuju organization: International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology – sequence: 7 givenname: Damien orcidid: 0000-0002-1664-2839 surname: Voiry fullname: Voiry, Damien organization: Institut Europeen des Membranes – sequence: 8 givenname: Sudip orcidid: 0000-0002-6765-2084 surname: Chakraborty fullname: Chakraborty, Sudip organization: Indian Institute of Technology (IIT) Indore – sequence: 9 givenname: Wenjing surname: Zhang fullname: Zhang, Wenjing organization: International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology – sequence: 10 givenname: Philip E surname: Batson fullname: Batson, Philip E organization: Rutgers University – sequence: 11 givenname: Leonard surname: Feldman fullname: Feldman, Leonard organization: Rutgers University – sequence: 12 givenname: Torgny surname: Gustafsson fullname: Gustafsson, Torgny organization: Rutgers University – sequence: 13 givenname: Manish surname: Chhowalla fullname: Chhowalla, Manish email: mc209@cam.ac.uk organization: International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31398001$$D View this record in MEDLINE/PubMed https://hal.umontpellier.fr/hal-02321715$$DView record in HAL |
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| Keywords | molybdenum disulfide single vacancy scanning transmission electron microscope hydrogen evolution reaction helium ion microscope |
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