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Title: A molecular cross-linking approach for hybrid metal oxides

Abstract

Developing methods to create hybrid materials to maximize their transformative capabilities has been the subject of significant interest. In particular, several key methods have been developed to manipulate earth abundant metal oxides such as TiO2 to produce hybrid materials with improved or new properties relevant to a broad spectrum of applications. Here, we introduce a new approach we refer to as “molecular doping”, whereby a hybrid molecular boron oxide material is formed from polyhedral boron cluster precursors of the type [B12(OH)12]2-. This new approach is enabled by the inherent robustness of the boron cluster molecular building block, which is compatible with harsh thermal and oxidizing conditions that are necessary for the synthesis of many metal oxides. In this work, we show how this material can be successfully interfaced with TiO2, resulting in boron-rich hybrid materials with unprecedented photophysical and electrochemical properties.

Authors:
 [1];  [2];  [3];  [1];  [2];  [4];  [2];  [2];  [2];  [2];  [5];  [2];  [6];  [7];  [2];  [2];  [8]; ORCiD logo [8]; ORCiD logo [2];  [9] more »; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [10];  [7];  [1];  [11];  [1];  [3]; ORCiD logo [1] « less
+ Show Author Affiliations
  1. Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry and Biochemistry, and California NanoSystems Inst. (CNSI)
  2. Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry and Biochemistry
  3. Univ. of California, Santa Barbara, CA (United States). Dept. of Chemical Engineering
  4. Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry and Biochemistry; Cairo Univ., Giza (Egypt)
  5. Univ. of California, Los Angeles, CA (United States). Dept. of Materials Science and Engineering
  6. Univ. of California, Santa Barbara, CA (United States). Materials Research Center
  7. Purdue Univ., West Lafayette, IN (United States). Davidson School of Chemical Engineering
  8. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  9. Univ. of Oregon, Eugene, OR (United States). Dept. of Chemistry and Biochemistry
  10. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS), X-ray Science Division
  11. Univ. of California, Los Angeles, CA (United States). Dept. of Chemistry and Biochemistry, and California NanoSystems Inst. (CNSI); Univ. of California, Los Angeles, CA (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1429806
Grant/Contract Number:  
AC02-06CH11357; 1532232; 1625776; ACI-1053575
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 17; Journal ID: ISSN 1476-1122
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Jung, Dahee, Saleh, Liban A. M., Berkson, Zachariah J., El-Kady, Maher F., Hwang, Jee Youn, Mohamed, Nahla, Wixtrom, Alex I., Titarenko, Ekaterina, Shao, Yanwu, McCarthy, Kassandra, Guo, Jian, Martini, Ignacio B., Kraemer, Stephan, Wegener, Evan C., Saint-Cricq, Philippe, Ruehle, Bastian, Langeslay, Ryan R., Delferro, Massimiliano, Brosmer, Jonathan L., Hendon, Christopher H., Gallagher-Jones, Marcus, Rodriguez, Jose, Chapman, Karena W., Miller, Jeffrey T., Duan, Xiangfeng, Kaner, Richard B., Zink, Jeffrey I., Chmelka, Bradley F., and Spokoyny, Alexander M. A molecular cross-linking approach for hybrid metal oxides. United States: N. p., 2018. Web. doi:10.1038/s41563-018-0021-9.
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Jung, Dahee, Saleh, Liban A. M., Berkson, Zachariah J., El-Kady, Maher F., Hwang, Jee Youn, Mohamed, Nahla, Wixtrom, Alex I., Titarenko, Ekaterina, Shao, Yanwu, McCarthy, Kassandra, Guo, Jian, Martini, Ignacio B., Kraemer, Stephan, Wegener, Evan C., Saint-Cricq, Philippe, Ruehle, Bastian, Langeslay, Ryan R., Delferro, Massimiliano, Brosmer, Jonathan L., Hendon, Christopher H., Gallagher-Jones, Marcus, Rodriguez, Jose, Chapman, Karena W., Miller, Jeffrey T., Duan, Xiangfeng, Kaner, Richard B., Zink, Jeffrey I., Chmelka, Bradley F., & Spokoyny, Alexander M. A molecular cross-linking approach for hybrid metal oxides. United States. https://doi.org/10.1038/s41563-018-0021-9
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Jung, Dahee, Saleh, Liban A. M., Berkson, Zachariah J., El-Kady, Maher F., Hwang, Jee Youn, Mohamed, Nahla, Wixtrom, Alex I., Titarenko, Ekaterina, Shao, Yanwu, McCarthy, Kassandra, Guo, Jian, Martini, Ignacio B., Kraemer, Stephan, Wegener, Evan C., Saint-Cricq, Philippe, Ruehle, Bastian, Langeslay, Ryan R., Delferro, Massimiliano, Brosmer, Jonathan L., Hendon, Christopher H., Gallagher-Jones, Marcus, Rodriguez, Jose, Chapman, Karena W., Miller, Jeffrey T., Duan, Xiangfeng, Kaner, Richard B., Zink, Jeffrey I., Chmelka, Bradley F., and Spokoyny, Alexander M. Mon . "A molecular cross-linking approach for hybrid metal oxides". United States. https://doi.org/10.1038/s41563-018-0021-9. https://www.osti.gov/servlets/purl/1429806.
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@article{osti_1429806,
title = {A molecular cross-linking approach for hybrid metal oxides},
author = {Jung, Dahee and Saleh, Liban A. M. and Berkson, Zachariah J. and El-Kady, Maher F. and Hwang, Jee Youn and Mohamed, Nahla and Wixtrom, Alex I. and Titarenko, Ekaterina and Shao, Yanwu and McCarthy, Kassandra and Guo, Jian and Martini, Ignacio B. and Kraemer, Stephan and Wegener, Evan C. and Saint-Cricq, Philippe and Ruehle, Bastian and Langeslay, Ryan R. and Delferro, Massimiliano and Brosmer, Jonathan L. and Hendon, Christopher H. and Gallagher-Jones, Marcus and Rodriguez, Jose and Chapman, Karena W. and Miller, Jeffrey T. and Duan, Xiangfeng and Kaner, Richard B. and Zink, Jeffrey I. and Chmelka, Bradley F. and Spokoyny, Alexander M.},
abstractNote = {Developing methods to create hybrid materials to maximize their transformative capabilities has been the subject of significant interest. In particular, several key methods have been developed to manipulate earth abundant metal oxides such as TiO2 to produce hybrid materials with improved or new properties relevant to a broad spectrum of applications. Here, we introduce a new approach we refer to as “molecular doping”, whereby a hybrid molecular boron oxide material is formed from polyhedral boron cluster precursors of the type [B12(OH)12]2-. This new approach is enabled by the inherent robustness of the boron cluster molecular building block, which is compatible with harsh thermal and oxidizing conditions that are necessary for the synthesis of many metal oxides. In this work, we show how this material can be successfully interfaced with TiO2, resulting in boron-rich hybrid materials with unprecedented photophysical and electrochemical properties.},
doi = {10.1038/s41563-018-0021-9},
journal = {Nature Materials},
number = ,
volume = 17,
place = {United States},
year = {Mon Mar 05 00:00:00 EST 2018},
month = {Mon Mar 05 00:00:00 EST 2018}
}
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https://doi.org/10.1038/s41563-018-0021-9
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Figures / Tables:

Figure 1 Figure 1: Overview of existing modification methods compared to molecular doping and preparation of molecularly doped TiO2 (3). a, Different approaches for the chemical modification of metal oxides. I, use of organic and inorganic dyes to sensitize metal oxide surfaces. II, elemental doping of metal oxides with light elements tomore » induce changes in their bulk properties. III, the introduction of defects in ordered crystalline metal oxides to change their optical properties. This work, molecular doping approach, whereby whole molecules are interfaced with metal oxides to effect changes in their photo- and electrochemical properties. b, Synthetic route towards the synthesis of material 3 utilizing the robust polyhedral boron cluster [NnBu4]2[1] as a key precursor. c, (left) Diffuse-reflectance UV-Vis data for material 3, plotted with data for TiO2 and Cs2[1] to highlight the dramatic difference in light absorption properties of all three materials; (right) simplified, non-rigorous cartoon model depicting the proposed structure of the hybrid molecular boron oxide material 3.« less
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