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1. Integrated halide perovskite photoelectrochemical cells with solar-driven water-splitting efficiency of 20.8%

Author

Fehr, Austin MK, Agrawal, Ayush, Mandani, Faiz, Conrad, Christian L, Jiang, Qi, Park, So Yeon, Alley, Olivia, Li, Bor, Sidhik, Siraj, Metcalf, Isaac, Botello, Christopher, Young, James L, Even, Jacky, Blancon, Jean Christophe, Deutsch, Todd G, Zhu, Kai, Albrecht, Steve, Toma, Francesca M, Wong, Michael, and Mohite, Aditya D

Subjects
Affordable and Clean Energy
Abstract

Achieving high solar-to-hydrogen (STH) efficiency concomitant with long-term durability using low-cost, scalable photo-absorbers is a long-standing challenge. Here we report the design and fabrication of a conductive adhesive-barrier (CAB) that translates >99% of photoelectric power to chemical reactions. The CAB enables halide perovskite-based photoelectrochemical cells with two different architectures that exhibit record STH efficiencies. The first, a co-planar photocathode-photoanode architecture, achieved an STH efficiency of 13.4% and 16.3 h to t60, solely limited by the hygroscopic hole transport layer in the n-i-p device. The second was formed using a monolithic stacked silicon-perovskite tandem, with a peak STH efficiency of 20.8% and 102 h of continuous operation before t60 under AM 1.5G illumination. These advances will lead to efficient, durable, and low-cost solar-driven water-splitting technology with multifunctional barriers.

Published
2023

2. Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen

Author

Xiong, Yihuang, Campbell, Quinn T., Fanghanel, Julian, Badding, Catherine K., Wang, Huaiyu, Kirchner-Hall, Nicole E., Theibault, Monica J., Timrov, Iurii, Mondschein, Jared S., Seth, Kriti, Katz, Rebecca, Villarino, Andres Molina, Pamuk, Betül, Penrod, Megan E., Khan, Mohammed M., Rivera, Tiffany, Smith, Nathan C., Quintana, Xavier, Orbe, Paul, Fennie, Craig J., Asem-Hiablie, Senorpe, Young, James L., Deutsch, Todd G., Cococcioni, Matteo, Gopalan, Venkatraman, Abruña, Hector D., Schaak, Raymond E., and Dabo, Ismaila

Subjects
Condensed Matter - Materials Science
Abstract

The production of hydrogen fuels, via water splitting, is of practical relevance for meeting global energy needs and mitigating the environmental consequences of fossil-fuel-based transportation. Water photoelectrolysis has been proposed as a viable approach for generating hydrogen, provided that stable and inexpensive photocatalysts with conversion efficiencies over 10% can be discovered, synthesized at scale, and successfully deployed (Pinaud et al., Energy Environ. Sci., 2013, 6, 1983). While a number of first-principles studies have focused on the data-driven discovery of photocatalysts, in the absence of systematic experimental validation, the success rate of these predictions may be limited. We address this problem by developing a screening procedure with co-validation between experiment and theory to expedite the synthesis, characterization, and testing of the computationally predicted, most desirable materials. Starting with 70,150 compounds in the Materials Project database, the proposed protocol yielded 71 candidate photocatalysts, 11 of which were synthesized as single-phase materials. Experiments confirmed hydrogen generation and favorable band alignment for 6 of the 11 compounds, with the most promising ones belonging to the families of alkali and alkaline-earth indates and orthoplumbates. This study shows the accuracy of a nonempirical, Hubbard-corrected density-functional theory method to predict band gaps and band offsets at a fraction of the computational cost of hybrid functionals, and outlines an effective strategy to identify photocatalysts for solar hydrogen generation.

Published
2021
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4. Emergent Degradation Phenomena Demonstrated on Resilient, Flexible, and Scalable Integrated Photoelectrochemical Cells

Author

Kistler, Tobias A, Zeng, Guosong, Young, James L, Weng, Lien‐Chun, Aldridge, Chase, Wyatt, Keenan, Steiner, Myles A, Solorzano, Oscar, Houle, Frances A, Toma, Francesca M, Weber, Adam Z, Deutsch, Todd G, and Danilovic, Nemanja

Subjects
Engineering, Materials Engineering, durability, on-sun testing, PEC cell scale-up, reproducibility, water splitting, Macromolecular and Materials Chemistry, Interdisciplinary Engineering, Macromolecular and materials chemistry, Materials engineering
Abstract

Photoelectrochemical (PEC) water splitting provides a pathway to generate sustainable clean fuels using the two most abundant resources on Earth: sunlight and water. Currently, most of the successful models of PEC cells are still fabricated on small scales near 1 cm2, which largely limits the mass deployment of solar-fuel production. Here, the scale-up to 8 cm2 of an integrated PEC (IPEC) device is demonstrated and its performance compared to a 1 cm2 IPEC cell, using state-of-the-art iridium and platinum catalysts with III–V photoabsorbers. The initial photocurrents at 1 sun are 8 and 7 mA cm−2 with degradation rates of 0.60 and 0.47 mA cm−2 day−1, during unbiased operation for the 1 and 8 cm2 devices, respectively. Evaluating under outdoor and indoor conditions at two U.S. National Laboratories reveals similar results, evidencing the reproducibility of this design's performance. Furthermore, the emerging degradation mechanisms during scale-up are investigated and the knowledge gained from this work will provide feedback to the broader community, since PEC device durability is a limiting factor in its potential future deployment.

Published
2020

5. Water Splitting: Emergent Degradation Phenomena Demonstrated on Resilient, Flexible, and Scalable Integrated Photoelectrochemical Cells (Adv. Energy Mater. 48/2020)

Author

Kistler, Tobias A, Zeng, Guosong, Young, James L, Weng, Lien‐Chun, Aldridge, Chase, Wyatt, Keenan, Steiner, Myles A, Solorzano, Oscar, Houle, Frances A, Toma, Francesca M, Weber, Adam Z, Deutsch, Todd G, and Danilovic, Nemanja

Subjects
Engineering, Chemical Sciences, Physical Chemistry, Affordable and Clean Energy, Macromolecular and Materials Chemistry, Materials Engineering, Interdisciplinary Engineering, Macromolecular and materials chemistry, Materials engineering
Published
2020

9. TiO2/TiN Interface Enables Integration of Ni5P4 Electrocatalyst with a III–V Tandem Photoabsorber for Stable Unassisted Solar-Driven Water Splitting

Author

Hwang, Shinjae, primary, Gu, Hengfei, additional, Young, James L., additional, Steiner, Myles A., additional, Laursen, Anders B., additional, Crichton, Ryan A., additional, Yeh, Yao-Wen, additional, Batson, Philip E., additional, Feldman, Leonard C., additional, Li, Mengjun, additional, Wyatt, Keenan, additional, Safari, Ahmad, additional, Deutsch, Todd G., additional, Garfunkel, Eric, additional, and Dismukes, G. Charles, additional

Published
2024
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16. Interfacial Connections between Organic Perovskite/n + Silicon/Catalyst that Allow Integration of Solar Cell and Catalyst for Hydrogen Evolution from Water

Author

Gu, Hengfei, primary, Zhang, Fei, additional, Hwang, Shinjae, additional, Laursen, Anders B., additional, Liu, Xin, additional, Park, So Yeon, additional, Yang, Mengjin, additional, Bramante, Rosemary C., additional, Hijazi, Hussein, additional, Kasaei, Leila, additional, Feldman, Leonard C., additional, Yeh, Yao‐Wen, additional, Batson, Philip E., additional, Larson, Bryon W., additional, Li, Mengjun, additional, Li, Yifei, additional, Wyatt, Keenan, additional, Young, James L., additional, Teeluck, Krishani, additional, Zhu, Kai, additional, Garfunkel, Eric, additional, and Dismukes, G. Charles, additional

Published
2023
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21. Interfacial Connections between Organic Perovskite/n+ Silicon/Catalyst that Allow Integration of Solar Cell and Catalyst for Hydrogen Evolution from Water.

Author

Gu, Hengfei, Zhang, Fei, Hwang, Shinjae, Laursen, Anders B., Liu, Xin, Park, So Yeon, Yang, Mengjin, Bramante, Rosemary C., Hijazi, Hussein, Kasaei, Leila, Feldman, Leonard C., Yeh, Yao‐Wen, Batson, Philip E., Larson, Bryon W., Li, Mengjun, Li, Yifei, Wyatt, Keenan, Young, James L., Teeluck, Krishani, and Zhu, Kai

Subjects
PHOTOCATHODES, SOLAR cells, TITANIUM nitride, ELECTROLYTIC corrosion, STANDARD hydrogen electrode, DIFFUSION barriers, PEROVSKITE
Abstract

The rapidly increasing solar conversion efficiency (PCE) of hybrid organic–inorganic perovskite (HOIP) thin‐film semiconductors has triggered interest in their use for direct solar‐driven water splitting to produce hydrogen. However, application of these low‐cost, electronic‐structure‐tunable HOIP tandem photoabsorbers has been hindered by the instability of the photovoltaic‐catalyst‐electrolyte (PV+E) interfaces. Here, photolytic water splitting is demonstrated using an integrated configuration consisting of an HOIP/n+silicon single junction photoabsorber and a platinum (Pt) thin film catalyst. An extended electrochemical (EC) lifetime in alkaline media is achieved using titanium nitride on both sides of the Si support to eliminate formation of insulating silicon oxide, and as an effective diffusion barrier to allow high‐temperature annealing of the catalyst/TiO2‐protected‐n+silicon interface necessary to retard electrolytic corrosion. Halide composition is examined in the (FA1‐xCsx)PbI3 system with a bandgap suitable for tandem operation. A fill factor of 72.5% is achieved using a Spiro‐OMeTAD‐hole‐transport‐layer (HTL)‐based HOIP/n+Si solar cell, and a high photocurrent density of −15.9 mA cm−2 (at 0 V vs reversible hydrogen electrode) is attained for the HOIP/n+Si/Pt photocathode in 1 m NaOH under simulated 1‐sun illumination. While this thin‐film design creates stable interfaces, the intrinsic photo‐ and electro‐degradation of the HOIP photoabsorber remains the main obstacle for future HOIP/Si tandem PEC devices. [ABSTRACT FROM AUTHOR]

Published
2023
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22. Failure Modes of Platinized pn⁺-GaInP Photocathodes for Solar-Driven H₂ Evolution

Author

Yu, Weilai, Buabthong, Pakpoom, Young, James L., Ifkovits, Zachary P., Byrne, Sean T., Steiner, Myles A., Deutsch, Todd G., and Lewis, Nathan S.

Abstract

The long-term stability for the hydrogen-evolution reaction (HER) of homojunction pn⁺-Ga_(0.52)In_(0.48)P photocathodes (band gap = 1.8 eV) with an electrodeposited Pt catalyst (pn⁺-GaInP/Pt) has been systematically evaluated in both acidic and alkaline electrolytes. Electrode dissolution during chronoamperometry was correlated with changes over time in the current density-potential (J–E) behavior to reveal the underlying failure mechanism. Pristine pn⁺-GaInP/Pt photocathodes yielded an open-circuit photopotential (Eoc) as positive as >1.0 V vs the potential of the reversible hydrogen electrode (RHE) and a light-limited current density (Jₚₕ) of >12 mA cm⁻² (1-sun illumination). However, Eₒ꜀ and Jₚₕ gradually degraded at either pH 0 or pH 14. The performance degradation was attributed to three different failure modes: (1) gradual thinning of the n⁺-emitter layer due to GaInP dissolution in acid; (2) active corrosion of the underlying GaAs substrate at positive potentials causing delamination of the upper GaInP epilayers; and (3) direct GaAs/electrolyte contact compromising the operational stability of the device. This work reveals the importance of both substrate stability and structural integrity of integrated photoelectrodes toward stable solar fuel generation.

Published
2022

26. Correction: Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen

Author

Xiong, Yihuang, primary, Campbell, Quinn T., additional, Fanghanel, Julian, additional, Badding, Catherine K., additional, Wang, Huaiyu, additional, Kirchner-Hall, Nicole E., additional, Theibault, Monica J., additional, Timrov, Iurii, additional, Mondschein, Jared S., additional, Seth, Kriti, additional, Katzbaer, Rowan R., additional, Villarino, Andrés Molina, additional, Pamuk, Betül, additional, Penrod, Megan E., additional, Khan, Mohammed M., additional, Rivera, Tiffany, additional, Smith, Nathan C., additional, Quintana, Xavier, additional, Orbe, Paul, additional, Fennie, Craig J., additional, Asem-Hiablie, Senorpe, additional, Young, James L., additional, Deutsch, Todd G., additional, Cococcioni, Matteo, additional, Gopalan, Venkatraman, additional, Abruña, Héctor D., additional, Schaak, Raymond E., additional, and Dabo, Ismaila, additional

Published
2022
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27. Understanding the Stability of Etched or Platinized p-GaInP Photocathodes for Solar-Driven H₂ Evolution

Author

Yu, Weilai, Young, James L., Deutsch, Todd G., and Lewis, Nathan S.

Abstract

The long-term stability in acidic or alkaline aqueous electrolytes of p-Ga_(0.52)In_(0.48)P photocathodes, with a band gap of ∼1.8 eV, for the solar-driven hydrogen-evolution reaction (HER) has been evaluated from a thermodynamic, kinetic, and mechanistic perspective. At either pH 0 or pH 14, etched p-GaInP electrodes corroded cathodically under illumination and formed metallic In0 on the photoelectrode surface. In contrast, under the same conditions, electrodeposition of Pt facilitated the HER kinetics and stabilized p-GaInP/Pt photoelectrodes against such cathodic decomposition. When held at 0 V versus the reversible hydrogen electrode, p-GaInP/Pt electrodes in either pH = 0 or pH = 14 exhibited stable current densities (J) of ∼−9 mA cm⁻² for hundreds of hours under simulated 1 sun illumination. During the stability tests, the current density–potential (J–E) characteristics of the p-GaInP/Pt photoelectrodes degraded due to pH-dependent changes in the surface chemistry of the photocathode. This work provides a fundamental understanding of the stability and corrosion mechanisms of p-GaInP photocathodes that constitute a promising top light absorber for tandem solar-fuel generators.

Published
2021

28. The Practicum Experience: Relic of the Sixties or Hope of the Eighties.

Author

De Young, James L.

Abstract

Practicum courses in theatre arts, which function as laboratories where students can practice theatre and receive academic credit for their efforts, greatly benefit students. Because the main goal of such practicums is cooperative achievement of the best production possible and since every step of a production involves a new problem or decision, the practicum course appears to provide an ideal model for life training as well as for artistic training. An experiential model created by Kolb, Chickering, and others tries to capture both the cognitive and the socioemotional factors that go into knowledge acquisition and application. The practicum theatre activities support this model by focusing on having experiences or taking actions, observing and reflecting on these experiences in order to generalize from them, and re-using the generalizations to solve new or similar problems. The direct experience that theatre practicums provide, therefore, assures strong student motivation because it teaches socialization skills and creative problem solving by offering students the experience of producing art and of plying their craft before an audience. (EL)

Published
1985

40. Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen

Author

Xiong, Yihuang, primary, Campbell, Quinn T., additional, Fanghanel, Julian, additional, Badding, Catherine K., additional, Wang, Huaiyu, additional, Kirchner-Hall, Nicole E., additional, Theibault, Monica J., additional, Timrov, Iurii, additional, Mondschein, Jared S., additional, Seth, Kriti, additional, Katzbaer, Rowan R., additional, Villarino, Andrés Molina, additional, Pamuk, Betül, additional, Penrod, Megan E., additional, Khan, Mohammed M., additional, Rivera, Tiffany, additional, Smith, Nathan C., additional, Quintana, Xavier, additional, Orbe, Paul, additional, Fennie, Craig J., additional, Asem-Hiablie, Senorpe, additional, Young, James L., additional, Deutsch, Todd G., additional, Cococcioni, Matteo, additional, Gopalan, Venkatraman, additional, Abruña, Héctor D., additional, Schaak, Raymond E., additional, and Dabo, Ismaila, additional

Published
2021
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48. Addressing the Stability Gap in Photoelectrochemistry: Molybdenum Disulfide Protective Catalysts for Tandem III–V Unassisted Solar Water Splitting

Author

Ben-Naim, Micha, primary, Britto, Reuben J., additional, Aldridge, Chase W., additional, Mow, Rachel, additional, Steiner, Myles A., additional, Nielander, Adam C., additional, King, Laurie A., additional, Friedman, Daniel J., additional, Deutsch, Todd G., additional, Young, James L., additional, and Jaramillo, Thomas F., additional

Published
2020
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49. Highly efficient and durable III–V semiconductor-catalyst photocathodes via a transparent protection layer

Author

Hwang, Shinjae, primary, Young, James L., additional, Mow, Rachel, additional, Laursen, Anders B., additional, Li, Mengjun, additional, Yang, Hongbin, additional, Batson, Philip E., additional, Greenblatt, Martha, additional, Steiner, Myles A., additional, Friedman, Daniel, additional, Deutsch, Todd G., additional, Garfunkel, Eric, additional, and Dismukes, G. Charles, additional

Published
2020
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