Spiro‐Phenothiazine Hole‐Transporting Materials: Unlocking Stability and Scalability in Perovskite Solar Cells

J Javier Urieta‐Mora (Departamento Química Orgánica Facultad C. C. Químicas Universidad Complutense de Madrid Av. Complutense s/n Madrid 28040 Spain) S Seung Ju Choi (Ulsan Advanced Energy Technology R&D Center Korea Institute of Energy Research 25 Techno Saneop‐ro 55beon‐gil, Nam‐gu Ulsan 44776 Republic of Korea) J Jaeki Jeong (Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering) S Silvia Orecchio (Departamento Química Orgánica Facultad C. C. Químicas Universidad Complutense de Madrid Av. Complutense s/n Madrid 28040 Spain) I Inés García‐Benito (Departamento Química Orgánica Facultad C. C. Químicas Universidad Complutense de Madrid Av. Complutense s/n Madrid 28040 Spain) M Manuel Pérez‐Escribano (Instituto de Ciencia Molecular Universidad de Valencia Catedrático José Beltrán 2 Paterna 46980 Spain) J Joaquín Calbo (Instituto de Ciencia Molecular, Universidad de Valencia, Catedrático José Beltrán 2, 46980 Paterna, Spain) L Likai Zheng (Institut des Sciences et Ingenierie Chimiques) M Minseop Byun (Ulsan Advanced Energy Technology R&D Center Korea Institute of Energy Research 25 Techno Saneop‐ro 55beon‐gil, Nam‐gu Ulsan 44776 Republic of Korea) S Seyeong Song (School of Energy and Chemical Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 South Korea) G Gi‐Hwan Kim (Department of Materials Engineering and Convergence Technology Gyeongsang National University Jinju 52828 Republic of Korea) S Shaik M. Zakeeruddin S Seog‐Young Yoon (School of Materials Science and Engineering Pusan National University Busan 46241 Republic of Korea) Y Yimhyun Jo (Ulsan Advanced Energy Technology R&D Center, Korea Institute of Energy Research, 25 Techno Saneop-ro 55beon-gil, Nam-gu, Ulsan 44776, Republic of Korea) A Agustín Molina‐Ontoria (Departamento Química Orgánica Facultad C. C. Químicas Universidad Complutense de Madrid Av. Complutense s/n Madrid 28040 Spain) E Enrique Ortí (Instituto de Ciencia Molecular, Universidad de Valencia, Catedrático José Beltrán 2, 46980 Paterna, Spain) N Nazario Martín (IMDEA Nanoscience, C/ Faraday 9 Campus De Cantoblanco Madrid Spain) M Michael Grätzel

Abstract

Abstract Improving both the efficiency and long‐term stability of perovskite solar cells (PSCs) is critical for their commercial deployment. Despite the widespread use of spiro‐OMeTAD as a hole‐transporting material (HTM), its inhomogeneous doping behavior and susceptibility to moisture and heat have hindered its large‐scale industrial implementation. Here, a family of spiro‐phenothiazine‐based HTMs (PTZ) is reported to address these drawbacks. Among them, the fluorene derivative (PTZ‐Fl) shows a larger Li + affinity and forms a compact interphase by intercalation in the perovskite passivating layer that prevents Li + migration. PSCs incorporating PTZ‐Fl exhibit power conversion efficiencies (PCEs) up to 25.8% (certified 25.2% under reverse scan), retaining 80% of their initial performance after 1000 h under ISOS‐L‐3 protocol. Furthermore, a 5 × 5 cm mini‐module reaches a PCE of 22.1%, surpassing spiro‐OMeTAD‐based PSCs and retaining over 85% of its efficiency after 1100 h under ISOS‐D‐1 protocol. These results demonstrate that PTZ‐Fl not only enables high PCEs but also substantially improves operational stability, offering a promising pathway toward the large‐scale deployment of next‐generation PSCs.

Article Details

Volume / Issue Vol. 1, Issue 1
Published July 28, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (18)

J

Javier Urieta‐Mora

Departamento Química Orgánica Facultad C. C. Químicas Universidad Complutense de Madrid Av. Complutense s/n Madrid 28040 Spain

S

Seung Ju Choi

Ulsan Advanced Energy Technology R&D Center Korea Institute of Energy Research 25 Techno Saneop‐ro 55beon‐gil, Nam‐gu Ulsan 44776 Republic of Korea

J

Jaeki Jeong

Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering

S

Silvia Orecchio

Departamento Química Orgánica Facultad C. C. Químicas Universidad Complutense de Madrid Av. Complutense s/n Madrid 28040 Spain

I

Inés García‐Benito

Departamento Química Orgánica Facultad C. C. Químicas Universidad Complutense de Madrid Av. Complutense s/n Madrid 28040 Spain

M

Manuel Pérez‐Escribano

Instituto de Ciencia Molecular Universidad de Valencia Catedrático José Beltrán 2 Paterna 46980 Spain

J

Joaquín Calbo

Instituto de Ciencia Molecular, Universidad de Valencia, Catedrático José Beltrán 2, 46980 Paterna, Spain

L

Likai Zheng

Institut des Sciences et Ingenierie Chimiques

M

Minseop Byun

Ulsan Advanced Energy Technology R&D Center Korea Institute of Energy Research 25 Techno Saneop‐ro 55beon‐gil, Nam‐gu Ulsan 44776 Republic of Korea

S

Seyeong Song

School of Energy and Chemical Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 South Korea

G

Gi‐Hwan Kim

Department of Materials Engineering and Convergence Technology Gyeongsang National University Jinju 52828 Republic of Korea

S

Shaik M. Zakeeruddin

S

Seog‐Young Yoon

School of Materials Science and Engineering Pusan National University Busan 46241 Republic of Korea

Y

Yimhyun Jo

Ulsan Advanced Energy Technology R&D Center, Korea Institute of Energy Research, 25 Techno Saneop-ro 55beon-gil, Nam-gu, Ulsan 44776, Republic of Korea

A

Agustín Molina‐Ontoria

Departamento Química Orgánica Facultad C. C. Químicas Universidad Complutense de Madrid Av. Complutense s/n Madrid 28040 Spain

E

Enrique Ortí

Instituto de Ciencia Molecular, Universidad de Valencia, Catedrático José Beltrán 2, 46980 Paterna, Spain

N

Nazario Martín

IMDEA Nanoscience, C/ Faraday 9 Campus De Cantoblanco Madrid Spain

M

Michael Grätzel