Improved performance and stability of photoelectrochemical water-splitting Si system using a bifacial design to decouple light harvesting and electrocatalysis

doi:10.1016/j.nanoen.2020.104478

Nano Energy

Volume 70, April 2020, 104478

https://doi.org/10.1016/j.nanoen.2020.104478 Get rights and content

Highlights

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Decoupling the light harvesting side from the electrocatalytic surface can nullify parasitic light absorption efficiently.
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The bifacial device demonstrated a high photocurrent density of 61.2 mA/cm² and an electrochemical stability of over 370 h.
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The omnidirectional light harvesting capability enables the device to absorb both direct and scattered sunlight effectively.

Abstract

Photoelectrochemical (PEC) splitting of water into hydrogen and oxygen is a promising way for the production of clean, and storable form of fuel but the PEC efficiency has remained low. Herein, we demonstrate enhanced light harvesting, charge carrier separation/transfer, and catalyst management with bifacial design for the Si-based photocathodes to achieve best-in-class hydrogen generation with excellent electrochemical stability. Decoupling the light harvesting side from the electrocatalytic surface nullifies parasitic light absorption and enables Si photocathodes that exhibit a photocurrent density of 39.01 mA/cm² and stability over 370 h in 1 M H₂SO₄(aq) electrolyte due to fully covered a 15 nm Pt without any intentional protective layer. Furthermore, the bifacial Si photocathode system with semi-transparent Pt layer of 5 nm developed herein are capable of collecting sunlight not only on the light harvesting side but also on the back side of the device, resulting in a photocurrent density of 61.20 mA/cm² under bifacial two-sun illumination, which yields 56.88% of excess hydrogen when compared to the monofacial PEC system. Combining the bifacial design with surface texturing and antireflection coating enables excellent omnidirectional light harvesting capability with a record hydrogen (photocurrent) generation, which provides a promising way to realize practical PEC water splitting applications.

Graphical abstract

Introduction

Photoelectrochemical (PEC) cells using light-absorbing materials as photoelectrodes mimicking natural photosynthesis to convert solar energy to a storable form of fuel have received significant attention [[1], [2], [3], [4]]. The overall PEC process consists of three parts: (i) light absorption and charge carrier generation; (ii) extraction of the excited carriers to the photoelectrode/electrolyte interface; and (iii) the hydrogen evolution reaction (HER) and oxygen evolution reactions (OER) over electrocatalysts [[3], [4], [5], [6]]. In order to effectively drive PEC water splitting, it is essential to harvest the majority of photons in the solar spectrum while also ensuring efficient charge separation/transfer and electrocatalysis [7]. Another key challenge in developing highly efficient photoelectrodes is the effective integration of electrocatalysts on the surface of the light absorbing material to lower the overpotential required to drive the water-splitting reaction [3,6,8]. In most cases, despite the excellent electrocatalytic activity, these catalysts absorb/reflect light resulting in a shadowing effect and reducing the light harvesting capability of the photoelectrode [[9], [10], [11], [12], [13]]. Moreover, PEC photoelectrodes made of high-performance solar absorbers, such as silicon and GaAs, are prone to corrosion in the electrolyte [[14], [15], [16], [17]], thus a corrosion-resistant protective layer on the surface of the photoelectrode is typically necessary. But this layer induces high surface resistivity and shadowing effects to inhibit charge carriers from the bulk of the semiconductor to the electrolyte [[17], [18], [19]].

Extensive research efforts on surface protection and passivation of Si-based photoelectrodes have been conducted, focusing on transparent and conducting materials, such as metals, metal oxides, and metal silicides deposited on the electrode surface [16,17,[20], [21], [22], [23], [24], [25]]. Overall, these studies have enhanced the stability and lifetime of Si photoelectrodes to some extent [[26], [27], [28], [29]], but not sufficiently for a functional prototype system. In addition to these efforts and promising results, PEC devices exhibiting both excellent bifacial light-capturing capability and long-term stability with efficient light-harvesting capabilities have not yet been demonstrated.

In current scenario, nearly all PEC photoelectrodes developed are monofacial, meaning that all the functionalities of the device, including light harvesting, electrocatalysis, and surface protection, are integrated on a single side of the PEC cell, resulting in the light harvesting side being overused while the back side of the device is underutilized (i.e., only for electrical connections) [4,30]. Engineering a photoelectrode to harvest the solar photons on both the front and back side of the device (atmospheric reflected photons) is an attractive strategy for enhancing the density of photo-generated carriers and the overall efficiency of PEC cells. In particular for PEC bifacial strategy is vital as Si serves as a photocathode in a dual photoelectrode configuration [31,32], in which most of the visible spectrum could be absorbed by the photoanode layer. Additionally, the important facts about bifacial photovoltaic (PV) device has been studied with energy efficiency gain plus equipment savings, extending durability, and enhancing albedo mechanically with additional yields of up to 25% are possible [33]. The bifacial PV devices is able to make more flexibility in photoelectrode designs for harvesting the omnidirectional solar irradiation from both the front and back surfaces, however, it has not been explored. Furthermore, the daily orbit of the sun changes the intensity and angle at which the direct component of the light impinges on the PEC cell. Therefore, omnidirectional light harvesting is a significant criterion for PV [[34], [35], [36]], and PEC devices to capture sunlight more efficiently throughout the day.

Here, we employed a new light decoupling scheme in which the top side of the photocathode is dedicated to the light harvesting, while the opposite side of the semi-transparent photocathode is used for the electrochemical reaction, abolishing the parasitic light absorption induced by the surface protection layer and electrocatalysts. By employing this decoupling scheme in n⁺np⁺-Si photocathode and fully covered 15 nm Pt catalyst, we achieved a saturation current density for HER (J_H, the current density at E⁰ = 0 V vs. RHE) of 39.01 mA/cm² and a stability of 370 h without any intentional protective layer under one sun illumination in 1 M H₂SO₄(aq) electrolyte — the highest combined current density and stability reported for a single junction Si-based photocathode. More importantly, we developed a silicon bifacial (SiBF) PEC photocathode with semi-transparent Pt layer of 5 nm which is able to absorb light on both sides of the device that achieves a record J_H of 61.20 mA/cm² at E⁰ = 0 V vs RHE and 56.88% of excess hydrogen (when compared with the monofacial devices) under bifacial illumination condition (one sun illumination on the light-harvesting (LH) side and one sun illumination on the Pt-coated side), which also shows excellent omnidirectional light harvesting characteristics. These results not only set a record for PEC water splitting based on Si photoelectrodes but also demonstrate the synergistic design of optical and catalytic components universally applied to all kinds of the photoelectrodes, which is crucial for advancing PEC hydrogen generation technology.

Section snippets

Bifacial photoelectrode design decoupling the light harvesting from electrocatalysis

Typically, surface protection layers and electrocatalysts deposited on top of the LH side of a PEC electrode lead to parasitic light absorption, which directly affects the light harvesting capability and efficiency of the device [[9], [10], [11], [12]]. Even though spatial decoupling of light absorption and electrocatalysis has been demonstrated in nanostructures with high aspect ratios [7,37,38], such designs are not fully decoupling scheme and complicated to implement with selective

Conclusion

We have demonstrated novel Si bifacial PEC cells with 5 nm semi-transparent Pt that feature a photocurrent density of 61.20 mA/cm² under bifacial illumination condition that yields 56.88% of excess H₂ generation when compared to the monofacial PEC system. The SiBF cells with efficient decoupling scheme employed herein is stable in corrosive acidic electrolyte for over 370 h using a pin-hole free of 15 nm Pt catalyst layer. Furthermore, multi-scale photon management using the bifacial

Bifacial Si cell fabrication

Micropyramids and microgrooves were fabricated on opposite sides of 300-μm-thick n-type (100) Si wafers (containing phosphorus as a dopant with 5 × 10¹⁵ cm⁻³ dopant concentration), separately. (i) For the LH side, the textured micropyramids were fabricated by dipping as-cut Si substrates in the anisotropic etching solution consisting of KOH, isopropyl alcohol, and H₂O for 20 min [36]. A p⁺-emitter layer (400 nm thick) was thermally diffused from the micropyramidal surface using a boron

Author contributions

H.C.Fu, P.V., and J.H.He designed the project, prepared samples, conducted experiments, analyzed the data and wrote the manuscript. M.L.T., W.J.L., Q.D., C.H.L., and S.J. assisted the PV and PEC experiments and analyzed the relevant data. M.B. and A.F. carried out the optical simulation. J.H.He supervised the project and directed the research. All authors commented on the paper.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

J.H.H. greatly acknowledges the baseline funding from King Abdullah University of Science and Technology (KAUST), KAUST Sensor Initiatives, KAUST Solar Center, and KAUST Catalysis Center. S.J. thanks the support from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under award DE-FG02-09ER46664.

Dr. Hui-Chun Fu received her Ph.D. degree from Electrical Engineering from King Abdullah University of Science and Technology (KAUST) with Prof. Jr-Hau He in 2019. She is currently carrying out her postdoctoral research with Prof. Song Jin at Chemistry, Wisconsin University. Her research focuses on the development of integrated photoelectrochemical system for simultaneous conversion and storage of intermittent solar energy. She made progress on the development of solar cells and photoelectrodes

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Dr. Purushothaman Varadhan received his PhD from Centre for Nanoscience and Nanotechnology, Bharathidasan University in 2014. He is the recipient of prestigious Australian Endeavor Fellowship in which he worked as a Postdoctoral Fellow in Australian National University, Australia till 2015. Later he moved to Nanoenergy group of Prof. Jr Hau He at King Abdullah University of Science and Technology (KAUST) where he works in the broad field of solar fuels. Most of his work is focused on the development of photoelectrochemical water-splitting system with technologically important semiconductors such as Si, and III-V for water-splitting, and CO₂ reduction.

Dr. Meng-Lin Tsai received his PhD degree from National Tsing Hua University, Taiwan in 2016. He worked as a postdoctoral research fellow at National Tsing Hua University from 2016 to 2017. He studied the fabrication of single atom tips, designing/maintaining ultrahigh vacuum systems, development of 2D devices, Si-organic hybrid solar cells, Si-based water splitting devices, III-V-based harsh electronics, and low-dimensional photodetectors. Dr. Tsai joined National Taiwan University of Science and Technology (NTUST) since August 2018 as an Assistant Professor. His research interests are low-temperature and large-scale growth of 2D materials and synthesis of air-stable inorganic perovskite quantum dots for display applications.

Dr. Wenjie Li received his B.S. in Chemistry from Fudan University in 2014. He earned his Ph.D. in Chemistry from University of Wisconsin-Madison in 2019, where he worked with Prof. Song Jin. His graduate research has been mainly focused on the understanding, development and demonstration of solar flow batteries (SFBs). Dr. Li is interested in studying the flow of electrons and ions through materials and interfaces and ways to control it, with a focus on energy conversion and storage applications.

Dr. Qi Ding received her bachelor degree in chemistry from Shandong University in 2011. She obtained her PhD in Department of Chemistry at University of Wisconsin-Madison in 2016 under the supervision of Prof. Song Jin. Her research interests include nanomaterial synthesis, characterization, and the development of catalyst and semiconductor systems for efficient solar-driven water splitting. Currently she works at PPG to develop novel technologies for paints, coatings and materials.

Dr. Chun-Ho Lin is currently a postdoctoral fellow in the University of New South Wales (UNSW). He received his Ph.D. degree in Electrical Engineering from King Abdullah University of Science and Technology (KAUST) in 2019. His research focuses on the development of halide perovskite-based optoelectronics using novel device design and contact engineering. His research actives also include perovskite lithography patterning, highly stable perovskite quantum dot papers, and flexible electronics.

Dr. Marcella Bonifazi is a PostDoc in the Physics Department at the University of Zurich. She took her PhD in Electrical Engineering, mainly focusing in the energy harvesting and clean energy production fields. She focused on projects about cost-efficient water desalination, photocatalysis and photoelectrochemical devices for water splitting and hydrogen generation purposes. Her main interest is introducing disorder and complexity in this field, exploiting nonlinear effects to model, optimize and improve performances of devices both from the theoretical and fabrication point of view.

Dr. Andrea Fratalocchi is Associate Professor (from July 2016) at KAUST University. In 2012 he became Editor of Nature Scientific Report. In 2017, he won the Middle East GCC Enterprise Award. In 2019, he was elected Fellow of the Institute of Physics (IOP), Senior Member of the IEEE, and Fellow of the Optical Society of America (OSA):

For pioneering innovations in the use of complex optical systems and the development of creative technologies in clean energy harvesting, bio-imaging, and advanced optical materials.

As in March 2019, Andrea Fratalocchi authored more than 150 articles, one book, two book chapters and four patents.

Dr. Song Jin received his B.S. from Peking University in 1997, Ph.D. in 2002 from Cornell University with Prof. Francis DiSalvo and carried out his postdoctoral research with Prof. Charles Lieber at Harvard University. Prof. Jin is interested in the chemistry, physics and technological applications of nanoscale and solid-state materials. Dr. Jin developed innovative synthesis of a variety of nanomaterials including metal chalcogenides, silicides, and halide perovskites, and discovered the screw dislocation-driven growth of nanomaterials. Jin advanced the exploitation of (nano)materials for electrocatalysis, solar energy conversion, energy storage, optoelectronics, nanospintronics, and biotechnology. He has authored over 200 publications and 8 patents.

Dr. Jr-Hau He is a Professor in Department of Materials Science and Engineering at City University of Hong Kong, Hong Kong. He has been a pioneer in optoelectronics, which reflects on his achievement of photon management on the light harvesting devices. He has conducted highly interdisciplinary researches to bridge those gaps between various research fields and between academia and industry. He is a Fellow of OSA, RSC and SPIE, and a senior member of IEEE. Visit his web for more information (nanoenergy.kaust.edu.sa).

¹: These authors contributed equally.

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Improved performance and stability of photoelectrochemical water-splitting Si system using a bifacial design to decouple light harvesting and electrocatalysis

Highlights

Abstract

Graphical abstract

Introduction

Section snippets

Bifacial photoelectrode design decoupling the light harvesting from electrocatalysis

Conclusion

Bifacial Si cell fabrication

Author contributions

Declaration of competing interest

Acknowledgements

Chem

Nano Energy

Nano Energy

Chem. Eng.

Sol. Energy Mater. Sol. Cells

Nano Energy

Nature

Acc. Chem. Res.

Chem. Mater.

Chem. Rev.

J. Phys. Chem. Lett.

Nat. Energy

J. Am. Chem. Soc.

Adv. Energy Mater.

ACS Energy Lett.

Nat. Mater.

Adv. Mater.

Energy Environ. Sci.

Adv. Energy Mater.

Science

Chem. Soc. Rev.