Sub-particle reaction and photocurrent mapping to optimize catalyst-modified photoanodes

Sambur, Justin B.; Chen, Tai-Yen; Choudhary, Eric; Chen, Guanqun; Nissen, Erin J.; Thomas, Elayne M.; Zou, Ningmu; Chen, Peng

doi:10.1038/nature16534

Title: Sub-particle reaction and photocurrent mapping to optimize catalyst-modified photoanodes

Journal Article · Wed Feb 03 00:00:00 EST 2016 · Nature (London)

DOI:https://doi.org/10.1038/nature16534· OSTI ID:1774980

Sambur, Justin B. ^[1]; Chen, Tai-Yen ^[1]; Choudhary, Eric ^[2]; Chen, Guanqun ^[1]; Nissen, Erin J. ^[3]; Thomas, Elayne M. ^[4]; Zou, Ningmu ^[1]; Chen, Peng ^[1]

Cornell Univ., Ithaca, NY (United States)
Cornell Univ., Ithaca, NY (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Colorado Mesa Univ., Grand Junction, CO (United States)
Univ. of Michigan, Ann Arbor, MI (United States)

The splitting of water photoelectrochemically into hydrogen and oxygen represents a promising technology for converting solar energy to fuel. The main challenge is to ensure that photogenerated holes efficiently oxidize water, which generally requires modification of the photoanode with an oxygen evolution catalyst (OEC) to increase the photocurrent and reduce the onset potential. However, because excess OEC material can hinder light absorption and decrease photoanode performance, its deposition needs to be carefully controlled—yet it is unclear which semiconductor surface sites give optimal improvement if targeted for OEC deposition, and whether sites catalysing water oxidation also contribute to competing charge-carrier recombination with photogenerated electrons. Surface heterogeneity exacerbates these uncertainties, especially for nanostructured photoanodes benefiting from small charge-carrier transport distances. In this study, we use super-resolution imaging, operated in a chargecarrier- selective manner and with a spatiotemporal resolution of approximately 30 nanometres and 15 milliseconds, to map both the electron- and hole-driven photoelectrocatalytic activities on single titanium oxide nanorods. We then map, with sub-particle resolution (about 390 nanometres), the photocurrent associated with water oxidation, and find that the most active sites for water oxidation are also the most important sites for charge-carrier recombination. Site-selective deposition of an OEC, guided by the activity maps, improves the overall performance of a given nanorod—even though more improvement in photocurrent efficiency correlates with less reduction in onset potential (and vice versa) at the subparticle level. Moreover, the optimal catalyst deposition sites for photocurrent enhancement are the lower-activity sites, and for onset potential reduction the optimal sites are the sites with more positive onset potential, contrary to what is obtainable under typical deposition conditions. These findings allow us to suggest an activity-based strategy for rationally engineering catalyst-improved photoelectrodes, which should be widely applicable because our measurements can be performed for many different semiconductor and catalyst materials.

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Research Organization:: Cornell Univ., Ithaca, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; US Army Research Office (ARO); National Science Foundation (NSF); Petroleum Research Foundation

Grant/Contract Number:: SC0004911; FG02-10ER16199; 63767-CH; 65814-CH; CBET-1263736; CHE-1137217; DMR-1063059; DMR-1120296; ECCS-15420819; 54289-ND7

OSTI ID:: 1774980

Journal Information:: Nature (London), Vol. 530, Issue 7588; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Nanoscale electrochemical kinetics & dynamics: the challenges and opportunities of single-entity measurements Edwards, M. A.; Robinson, D. A.; Ren, H. Faraday Discussions, Vol. 210 https://doi.org/10.1039/c8fd00134k	journal	January 2018
Direct SERS tracking of a chemical reaction at a single 13 nm gold nanoparticle Zhang, Kun; Liu, Yujie; Wang, Yuning Chemical Science, Vol. 10, Issue 6 https://doi.org/10.1039/c8sc04496a	journal	January 2019
Advanced space- and time-resolved techniques for photocatalyst studies Gao, Yuying; Nie, Wei; Wang, Xiuli Chemical Communications, Vol. 56, Issue 7 https://doi.org/10.1039/c9cc07128h	journal	January 2020
Construction of a triple sequential junction for efficient separation of photogenerated charges in photocatalysis Li, Chun; Yang, Xia; Chen, Xuebing Chemical Communications, Vol. 56, Issue 2 https://doi.org/10.1039/c9cc08013a	journal	January 2020
Rational design of functional materials guided by single particle chemiluminescence imaging Kong, Weijun; Li, Qi; Wang, Wei Chemical Science, Vol. 10, Issue 21 https://doi.org/10.1039/c9sc00954j	journal	January 2019
Single nanoparticle photoelectrochemistry: What is next? Wang, Li; Schmid, Merranda; Sambur, Justin B. The Journal of Chemical Physics, Vol. 151, Issue 18 https://doi.org/10.1063/1.5124710	journal	November 2019
Intermittent photocatalytic activity of single CdS nanoparticles Fang, Yimin; Li, Zhimin; Jiang, Yingyan Proceedings of the National Academy of Sciences, Vol. 114, Issue 40 https://doi.org/10.1073/pnas.1708617114	journal	September 2017
Direct high-resolution mapping of electrocatalytic activity of semi-two-dimensional catalysts with single-edge sensitivity Sun, Tong; Wang, Dengchao; Mirkin, Michael V. Proceedings of the National Academy of Sciences https://doi.org/10.1073/pnas.1821091116	journal	May 2019
Single-molecule and -particle probing crystal edge/corner as highly efficient photocatalytic sites on a single TiO ₂ particle Wang, Wei-Kang; Chen, Jie-Jie; Lou, Zai-Zhu Proceedings of the National Academy of Sciences, Vol. 116, Issue 38 https://doi.org/10.1073/pnas.1907122116	journal	September 2019
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Roadmap on plasmonics Stockman, Mark I.; Kneipp, Katrin; Bozhevolnyi, Sergey I. Journal of Optics, Vol. 20, Issue 4 https://doi.org/10.1088/2040-8986/aaa114	journal	March 2018
Tunable dextran retention of MXene-TiO ₂ mesoporous membranes by adjusting the 2D MXene content Sun, Yuqing; Xu, Zhi; Zhuang, Yongxiang 2D Materials, Vol. 5, Issue 4 https://doi.org/10.1088/2053-1583/aad01e	journal	July 2018
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Correlated Single-Molecule Reaction Imaging and Photocurrent Measurements Reveal Underlying Rate Processes in Photoelectrochemical Water Splitting Sambur, Justin B.; Shepherd, Douglas P.; Hesari, Mahdi Journal of The Electrochemical Society, Vol. 166, Issue 5 https://doi.org/10.1149/2.040195jes	journal	January 2019
Indium Tin-Oxide Wrapped 3D rGO and TiO2 Composites: Development, Characterization, and Enhancing Photocatalytic Activity for Methylene Blue Gong, Cheng; Xu, Shiyin; Xiao, Peng Catalysts, Vol. 9, Issue 10 https://doi.org/10.3390/catal9100848	journal	October 2019
Efficiency and Bond Selectivity in Plasmon-Induced Photochemistry Cortés, Emiliano Advanced Optical Materials, Vol. 5, Issue 15 https://doi.org/10.1002/adom.201700191	journal	June 2017
Observing the Reversible Single Molecule Electrochemistry of Alexa Fluor 647 Dyes by Total Internal Reflection Fluorescence Microscopy Fan, Sanjun; Webb, James E. A.; Yang, Ying Angewandte Chemie International Edition, Vol. 58, Issue 41 https://doi.org/10.1002/anie.201907298	journal	August 2019
Plasmonic hot electron transport drives nano-localized chemistry Cortés, Emiliano; Xie, Wei; Cambiasso, Javier Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14880	journal	March 2017
Charge separation via asymmetric illumination in photocatalytic Cu2O particles Chen, Ruotian; Pang, Shan; An, Hongyu Nature Energy, Vol. 3, Issue 8 https://doi.org/10.1038/s41560-018-0194-0	journal	July 2018
The 2018 correlative microscopy techniques roadmap Ando, Toshio; Bhamidimarri, Satya Prathyusha; Brending, Niklas Universität des Saarlandes https://doi.org/10.22028/d291-29241	collection	January 2018
Tunneling Mode of Scanning Electrochemical Microscopy: Probing Electrochemical Processes at Single Nanoparticles Sun, Tong; Wang, Dengchao; Mirkin, Michael V. Angewandte Chemie International Edition, Vol. 57, Issue 25 https://doi.org/10.1002/anie.201801115	journal	May 2018
Total Internal Reflection-Based Extinction Spectroscopy of Single Nanoparticles Li, Meng; Yuan, Tinglian; Jiang, Yingyan Angewandte Chemie, Vol. 131, Issue 2 https://doi.org/10.1002/ange.201810324	journal	November 2018
Observing the Reversible Single Molecule Electrochemistry of Alexa Fluor 647 Dyes by Total Internal Reflection Fluorescence Microscopy Fan, Sanjun; Webb, James E. A.; Yang, Ying Angewandte Chemie, Vol. 131, Issue 41 https://doi.org/10.1002/ange.201907298	journal	August 2019
Rationalizing Acid Zeolite Performance on the Nanoscale by Correlative Fluorescence and Electron Microscopy Van Loon, Jordi; Janssen, Kris P. F.; Franklin, Thomas ACS Catalysis, Vol. 7, Issue 8 https://doi.org/10.1021/acscatal.7b01148	journal	July 2017
Bimetallic Effect of Single Nanocatalysts Visualized by Super-Resolution Catalysis Imaging Chen, Guanqun; Zou, Ningmu; Chen, Bo ACS Central Science, Vol. 3, Issue 11 https://doi.org/10.1021/acscentsci.7b00377	journal	November 2017
Single Molecule Nanospectroscopy Visualizes Proton-Transfer Processes within a Zeolite Crystal Ristanović, Zoran; Kubarev, Alexey V.; Hofkens, Johan Journal of the American Chemical Society, Vol. 138, Issue 41 https://doi.org/10.1021/jacs.6b06083	journal	October 2016
Reversible and Site-Dependent Proton-Transfer in Zeolites Uncovered at the Single-Molecule Level Ristanović, Zoran; Chowdhury, Abhishek Dutta; Brogaard, Rasmus Y. Journal of the American Chemical Society, Vol. 140, Issue 43 https://doi.org/10.1021/jacs.8b08041	journal	October 2018
Ultrathin Hematite Photoanode with Gradient Ti Doping Liu, Pengfei; Wang, Chongwu; Wang, Lijie Research, Vol. 2020 https://doi.org/10.34133/2020/5473217	journal	January 2020

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