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Visible-to-near-infrared light-harvesting A-π-D-π-A porphyrins, ZnP-CPDT and ZnP-BT are proved to be highly efficient in photocatalytic hydrogen evolution (PHE) with the highest PHE rate (ηH2) of 1.80 mmol g−1 h−1 for ZnP-CPDT.

Wide-bandgap perovskites as a class of promising top-cell materials have shown great promise in constructing efficient perovskite-based tandem solar cells, but their intrinsic relatively low radiative efficiency results in a large open-circuit voltage (

Development of water-stable metal-organic frameworks (MOFs) for promising visible-light-driven photocatalytic water splitting is highly desirable but still challenging. Here we report a novel p-type nickel-based MOF single crystal (Ni-TBAPy-SC) and its exfoliated nanobelts (Ni-TBAPy-NB) that can bear a wide range of pH environment in aqueous solution. Both experimental and theoretical results indicate a feasible electron transfer from the H

A new Ir-complex conjugated porphyrin exhibits AIE property for the Ir-complex unit, inhibition of ACQ of the porphyrin unit and efficient energy transfer from the Ir-complex to the porphyrin, therefore, enhanced photocatalytic H2 evolution.

Naphthalimide (NI) conjugated Pt(ii)-porphyrins show high performances in cocatalyst-free photocatalytic hydrogen evolution (PHE) because of their long-lived excited states and strong light-harvesting capability.

Lead-free hybrid perovskites (LFHPs) have sparked considerable research interest in photocatalysis. This review introduces the surface engineering and photophysical behaviors of LFHPs for diverse solar-induced photocatalytic applications.

Organic dyes, porphyrins and inorganic complexes containing imidazole (IM) motifs have been demonstrated as a new class of sensitizers in dye-sensitized solar cells (DSSCs). Particularly, the amphoteric nature of IM-based motifs allows them to be used as donors (D), auxiliary donors (D

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A simple heteroleptic iridium(III) photosensitizer, Ir-1, containing two ligands 5-(trifluoromethyl)-2-phenylpyridine (ĈN–CF3) and bipyridine (NN) has for the first time been studied for cocatalys...

Luminescent copper(I) halide complexes with bi- and tridentate rigid ligands have gained wide research interests. In this paper, six tetracoordinate dinuclear copper(I) halide complexes, Cu2X2(ppda)2 [ppda = 2-[2-(dimethylamino)phenyl(phenyl)phosphino]-N,N-dimethylaniline, X = I (1), Br (2), Cl (3)] and Cu2X2(pfda)2 [pfda = 2-[2-(dimethylamino)-4-(trifluoromethyl)phenyl(phenyl)phosphino]-N,N-dimethyl-5-trifluoromethylaniline, X = I (4), Br (5), Cl (6)], were successfully prepared and systematically characterized on their structures and photophysical properties. Complexes 1-5 have a centrosymmetric form with a planar Cu2X2 unit, and complex 6 has a mirror symmetry form with a butterfly-shaped Cu2X2. Solid complexes 1, 4, and 5 emit delayed fluorescence at room temperature, intense blue to greenish yellow (λmax = 443-570 nm) light, and their peak wavelengths are located at 443-570 nm with microsecond lifetimes (τ = 0.4-19.2 μs, ΦPL = 0.05-0.48). Complexes 2, 3, and 6 show prompt fluorescence, very weak yellowish green to yellow (λmax = 534-595 nm) emission with peak wavelengths at 534-595 nm, and lifetimes in nanoseconds (τ = 4.4-9.3 ns, ΦPL < 0.0001). (Metal + halide) to ligand and intraligand charge transitions are the main origin of the emission of the complexes. Solution-processed, complex-4-based nondoped and doped devices emit yellow green light with CIE coordinated at (0.41, 0.51), a maximum EQE up to 0.17%, and luminance reaching 75.52 cd/m2.

The synthesis of conjugated polymers specifically for organic electrochemical transistors (OECTs) has attracted much attention recently for their great potential in biological applications. In this case, not only the carrier mobility but also the ionic conduction capability and redox stability of the polymers in an aqueous environment are critical to the device performance. Here, we report a series of dithienyldiketopyrrolopyrrole (DTDPP) based polymers used in organic electrochemical transistors (OECTs). With the combination of ethylenedioxythiophene (EDOT) and glycolated side chains, the optimized polymers present low ionization potential and ultrahigh volumetric capacitance. The resultant OECTs show high transconductance, a high on/off ratio, low threshold voltage, fast response time and remarkably high stability in aqueous solutions. Furthermore, various short-term synaptic functions are successfully mimicked through the optimization of electrolytes and operation modes, indicating that the DPP-based polymer is promising for broad applications in bioelectronics.

A uniform nickel film could be coated on crown ether-modified carbon nanotubes (c-CNTs) by electroless deposition. The products CNT@Ni and c-CNT@Ni were oxidized and compressed into CNT@Ni@(NiOH)2 and c-CNT@Ni@(NiOH)2 discs, respectively. The areal and volumetric capacitances of CNT@Ni@(NiOH)2 and c-CNT@Ni@(NiOH)2 were compared and c-CNT@Ni@(NiOH)2 showed a lower resistance.

Organic solar cells (OSCs) have been considered as a promising, cost-effective alternative to the silicon-based solar cells due to their light weight, mechanical flexibility, and easy fabrication features. Over the past decades, organic semiconducting materials have been developed rapidly for use in bulk heterojunction (BHJ) OSCs. Among them, porphyrin-based small molecules have been widely applied as electron donors and electron acceptors in BHJ OSCs due to their large conjugated planar structures and strong UV-visible and near-infrared absorption. In this short review article, we mainly focus on summarizing the recent progress of the rational design of push–pull porphyrin-based small molecules for BHJ OSC applications. After various structural developments, the power conversion efficiencies (PCEs) of porphyrin-based small molecules as electron donors in OSCs have exceeded 12%. Apart from that, a PCE of 9.6% has been recorded for a device based on a porphyrin electron acceptor. This paper will provide a good insight into the structure–performance correlation and molecular engineering strategies of porphyrin-based small molecules in a stepwise manner.

Photocatalytic hydrogen evolution (PHE) is a promising strategy to produce environmentally friendly clean energy with the use of solar power and water. For this, developing an efficient and noble metal free photocatalytic system (PS) comprising high light-harvesting and photostable photosensitizers is an important and challenging task. Herein, a new porphyrin photosensitizer ZnDC(p-NI)PP, containing two naphthalimide (NI) donor chromophores and 4-carboxyphenyl substituents is developed for PHE. Using chloropyridinecobaloxime (CoPyCl) as a cocatalyst in phosphate buffer/THF solution at pH 7.4, the homogeneous PS of ZnDC(p-NI)PP exhibits a very high hydrogen evolution rate (ηH2) of 35.70 mmol g−1 h−1, turnover number (TON) of 5958 and apparent quantum efficiency (AQE) of 10.01%. This performance recorded under the same conditions is significantly higher than that of the PS of ZnDCPP which lacks the NI moieties (ηH2 of 4.64 mmol g−1 h−1, TON of 1397 and AQE of 1.30%), the typical PS of ZnTCPP with four 4-carboxyphenyl substituent groups (ηH2 of 2.43 mmol g−1 h−1, TON of 562 and AQE of 1.00%), and previously reported ZnD(p-NI)PP containing only two NI chromophores (ηH2 of 3.8 mmol g−1 h−1, TON of 590 and AQE of 1.5%). The noticeable performance of ZnDC(p-NI)PP in PHE is attributed to the intramolecular energy transfer from the NI donor chromophore to the porphyrin acceptor that would promote the long-lived photoexcitation states. At the same time, the anionic form (–COO−) of 4-carboxyphenyl substituents at pH 7.4 enables a faster electron transfer from the porphyrin group to the cationic Co(III) due to electrostatic force. To the best of our knowledge, the PHE results of ZnDC(p-NI)PP represent the best one for porphyrin photosensitizers and cobaloxime PSs reported so far. This work paves a new direction for developing new porphyrin-based materials for efficient PHE through facile molecular structure engineering.

The development of near-infrared (NIR)-absorbing nanoagents for personalized multifunctional phototheranostics has attracted considerable attention in the past decade. Recently, the organic nanomaterials with good biosafety are considered as promising phototheranostic agents, while their facile synthesis remains challenging. Inspired by the preparation of carbon nanodots, we fabricate the NIR-absorbing phthalocyanine-based nanodots (ZnPc-NDs) using a facile method for multifunctional phototheranostics. The significant aggregation of phthalocyanines in nanodots induces a complete fluorescence quenching, which affords a high photothermal conversion efficiency (η = 45.7%). The ZnPc-NDs disperse very well in water media with an average diameter around 80 nm. Further conjugation of biotin on the surface of ZnPc-NDs affords tumor-targeting phthalocyanine nanodots (ZnPc-BT). The ZnPc-BT are demonstrated with favorable biocompatibility, intense photoacoustic signals, high tumor accumulation, and effective tumor suppression in vivo. This Article provides a new insight for further developing nanomedicines with imaging and therapeutic functions to treat cancers precisely and effectively.

We employ facile aromatic nucleophilic substitution between the mercapto (-SH) and arylfluoro (Ar-F) groups to achieve extensive and robust cross-linking of a coordination host by porphyrin guests that also serve the purpose of versatile postsynthetic functionalization. For this, a tritopic linker with three trident-like thiol-flanked carboxyl units are reacted with ZrOCl

Two new A-D-A small-molecule donors (C8T-BDTDP and C8ST-BDTDP) are prepared from benzodithiophene (BDT)-linked dimeric porphyrin (DP), which differ in side chains of BDT linkers with 4,8-bis[5-(2-ethylhexyl)thiophen-2-yl]benzo[1,2-b:4,5-b']dithiophene (C8T-BDT) for the former and 4,8-bis{5-[(2-ethylhexyl)thio]-2-thienyl}benzo[1,2-b:4,5-b']dithiophene (C8ST-BDT) for the latter. Both dimeric porphyrin donors show strongly UV-visible to near-infrared absorption. Compared to C8T-BDTDP, C8ST-BDTDP with an alkylthiothienyl-substituted BDT linker exhibits more intense absorption bands in the film and a lower highest occupied molecular orbital energy level. The blend film of the electron acceptor 6TIC with the respective dimeric porphyrin donor displays a broad photon response from 400 to 900 nm, unfortunately, with an absorption valley at ca. 600 nm. The device based on C8ST-BDTDP/6TIC demonstrates a promising power conversion efficiency (PCE) of 10.39% with a high short-circuit current density (

A linear 5,15-di(naphthalimide) substituted porphyrin ZnD(p-NI)PP is facilely self-assembled into nanowires in solid with well-defined morphology through the synergistic π–π stack interactions of b...

Carbon dots (CDs) as an emerging type of carbon nanomaterials exhibit great potential in bioimaging applications owing to their superior optical properties and excellent biocompatibility. However, ...

A series of metallopolymers containing two lanthanides (Poly-Eu-Tb, molar ratio of Eu3+/Tb3+ = 1 : 1, 1 : 2, 1 : 4 and 1 : 8) have been synthesized via the coordination of Eu3+ and Tb3+ ions to terpyridine-based polymers (Poly). At a high concentration (1 mg mL−1) in DMF, Poly-Eu-Tb with an optimal Eu3+/Tb3+ ratio (1 : 8) shows strong white light emission from the Poly backbone and Eu3+ and Tb3+ ions, but changes to very weak blue emission mainly from the Poly backbone when diluted to an extremely low concentration (0.1 mg mL−1). For typical aggregation-induced-emission (AIE) effects, a strong white light emission can be recovered along with the addition of 1,4-dioxane to the diluted DMF solution. Moreover, Poly-Eu-Tb is uniformly dispersed on the surface of cellulose nanopaper (CNFs) via a simple solution coating process, giving a new flexible cellulose nanopaper Poly-Eu-Tb-CNFs. The new cellulose nanopaper characteristic of UV-excited white light emission shows excellent haze properties (haze value as high as 98%) and therefore could be applied as a substrate and light diffuser in the fabrication of soft-white-light emitting diodes (SWLEDs).

Two new iridium motif linked porphyrins, MBPyZnP-Ir and TBPyZnP-Ir are developed for photocatalytic hydrogen evolution (PHE). The tetra-iridium linked one, TBPyZnP-Ir, displayed the highest H2 production rate (ηH2) of 16.12 mmol g−1 h−1 within 5 h of irradiation, which is over 2.73-fold higher than MBPyZnP-Ir (5.90 mmol g−1 h−1) and much higher than their precursors TBPyZnP (0.12 mmol g−1 h−1) and MBPyZnP (0.06 mmol g−1 h−1) without iridium. The superior ηH2 of TBPyZnP-Ir could be explained by the iridium motifs linked to the porphyrin, stabilizing the triplet states of the porphyrin through intramolecular energy transfer; thus enhancing electron transfer from the triplet photo-excited porphyrin moiety to the cobaloxime co-catalyst and consequently proton reduction.

More efficient intramolecular energy transfer in the naphthalimide–porphyrin complex, ZnT(p-NI)TP, is accomplished by an electron rich coplanar thiophene π-linkage compared to the analogous porphyrin ZnT(p-NI)PP bearing a less coplanar phenylene π-linker. As a result, ZnT(p-NI)TP shows enhanced light-harvesting ability, electron lifetime and photoinduced charge carrier separation compared to ZnT(p-NI)PP and this boosted electron transfer from the photoexcited porphyrin moiety to the proton reduction catalyst, consequently, resulting in a 2.9 fold higher hydrogen evolution rate (ηH2) of ZnT(p-NI)TP (4.28 mmol g−1 h−1) than ZnT(p-NI)PP (1.50 mmol g−1 h−1). ZnT(p-NI)TP is also much more photostable than ZnT(p-NI)PP and continued to show hydrogen evolution for up to 50 h.

Two new A2–π–D–A1–D–π–A2 structural porphyrin small molecules denoted as TDPP-2P and ETDPP-2P are constructed from dimeric porphyrin centers, in which the two porphyrin moieties are linked by either the electron deficient 3,6-di(thiophen-2-yl)pyrrolo[3,4-c]pyrrole-1,4(2H,5H)-dione (TDPP) for the former, or diethynyl substituted TDPP for the latter, further symmetrically π-extended with electron withdrawing rhodanine units through phenylenethynylene π-bridges. For both, 2-butyloctyl and 1-octylundecyl branched alkyl chains are attached to TDPP and porphyrin moieties, respectively, to improve their solubility and self-assembly properties. Compared to TDPP-2P, ETDPP-2P shows a broader absorption in the near-infrared (NIR) range over 1000 nm due to the enhanced coplanarity of the dimeric porphyrin center. Using IT-M as the acceptor, the blend film ETDPP-2P:IT-M accomplishes a panchromatic photoresponse from 300–900 nm, and as a result, the device exhibits a prominent PCE of 5.69%, whereas, the film TDPP-2P:IT-M shows a lower PCE of 4.12% due to the lack of NIR photoresponses. These primary results open up a promising avenue for constructing porphyrin-based all small molecule organic solar cells with a panchromatic photoresponse.

Donor–acceptor two-dimensional covalent organic frameworks, PD-COF-23 and PD-COF-23-Ni, are constructed and applied for selective CO2 reduction with CO conversion rates of 20.9 μmol g−1 h−1 and 40.0 μmol g−1 h−1, respectively, in the absence of any additional photosensitizers and noble metal co-catalysts within an operation time of 25 h. The multilayer nanosheet structure, efficient charge separation and transport, and internal reductive quenching cycle of the NiTAPP fragments of PD-COF-23-Ni result in its higher photocatalytic efficiency than that of PD-COF-23.

Photothermal agents can transfer the absorbed light to heat energy, offering a noninvasive and controllable method to kill tumor cells and tissues. Here, we develop a simple and high-output strategy to prepare photothermal nanodots (MnPc-NDs) by the self-assembly and carbonization of manganese phthalocyanine. The aggregation of phthalocyanine molecules in the nanodots induces an efficient photothermal conversion. Thanks to the high thermal stability of phthalocyanine, the macrocycle is well preserved in the core of nanodots under the controlled hydrothermal temperature. Moreover, the as-prepared MnPc-NDs disperse well in aqueous solution with an average nanoscale size around 60 nm. The intense absorption in near-infrared (NIR) region, along with efficient reactive oxygen generation, high photothermal conversion efficiency (η = 59.8%), and excellent magnetic resonance contrast performances of MnPc-NDs endow them with great potential for MRI-guided cancer phototherapy. Therefore, the contribution provides a facile way to develop theranostic MnPc-NDs for precise and efficient cancer imaging and therapy.

To explore the effect of the introduction of heteroatoms on the properties of porphyrin materials, a new porphyrin-based derivative small-molecule donor named as PorTT-T was designed and synthesized based on alkyl-thieno[3,2-b]thiophene(TT)-substituted porphyrins. The linker bridge and end groups of PorTT-T were the same as those of XLP-II small-molecule donor materials, while the side-chain attached to the core of thieno[3,2-b]thiophene(TT)-substituted porphyrin was different. Measurements of intrinsic properties showed that PorTT-T has wide absorption and appropriate energy levels in the UV-visible range. A comparison of the morphologies of the two materials using atomic force microscopy showed that PorTT-T has a better surface morphology with a smaller root-mean-square roughness, and can present closer intermolecular stacking as compared to XLP-II. The device characterization results showed that PorTT-T with the introduced S atom has a higher open circuit voltage of 0.886 eV, a higher short circuit current of 12.03 mAcm−2, a fill factor of 0.499, a high photovoltaic conversion efficiency of 5.32%, better external quantum efficiency in the UV-visible range, and higher hole mobility.

Three new molecular A-π-D-π-A type donors, P1, P2 and P3, comprising an alkylthiothienyl substituted porphyrin electron donor core (D) and two 3-ethylrhodanine electron acceptor moieties (A) connected peripherally to the porphyrin core via respectively a monomeric, dimeric or trimeric phenylethynyl π-linkage, are synthesized and studied for their optoelectronic, charge transport, and photovoltaic properties. The hole mobilities of their blend films with PC71BM follow the order of P3> P2 > P1 in hole-only device. When used as electron donors with fullerene acceptor, PC71BM, in conventional bulk heterojunction organic solar cells, the optimal device with P1 donors shows a lower FF, but an intensity stronger and broader EQE, the highest JSC and VOC. As a whole, the PCEs of their optimal devices follow the order of P1> P2 > P3, corresponding to 8.61%, 8.20% and 7.82%, respectively. These results clearly demonstrate the decisive influence of π–linkage length over photovoltaic performance, and that the shorter the π–linkage length the better the photovoltaic performance.

In this study, a polymerizable terpyridine 2-(4-(4-(4-vinylbenzyloxy)phenyl)-6-(pyridin-2-yl)pyridin-2-yl)pyridine was synthesized, with N-(2-hydroxyethyl)acrylamide (HEAA) used to obtain an amphipathic polymer (Poly) through free radical polymerization. Then, Poly was coordinated with LnCl3 or Ln(ABM)3(H2O)2 (ABM = 4,4,4-trifluoro-1-phenylbutane-1,3-dione; Ln = Eu or Gd) in an equimolar ratio and a series of terpyridine-based Ln(III)-metallopolymer Poly-Eu or Poly-Eu-ABM obtained. The results strongly suggested that Poly-Eu exhibited aggregation-induced lanthanide emission. In contrast, after the introduction of a secondary sensitizer, ABM to Poly-Eu, aggregation-caused quenching effects were observed in Poly-Eu-ABM. In addition, both Poly-Eu and Poly-Eu-ABM were applied as fluorescence sensors to selectively detect pyrophosphate (PPi) among a series of different anions and the detection limit found to be at the nanomolar scale. Furthermore, high PPi sensitivity and selectively, low toxicity, and water solubility of this metallopolymer matrix Poly-Eu-ABM were used to detect PPi in living cells.

This study examines the correlation between the structure of four perylenediimide (PDI) derivatives and their optoelectronic behaviors. Three of them with one, two or four PDI moieties conjugated peripherally to porphyrin core by phenylene linker, denoted as nPDI-ZnP (n = 1,2,4), are investigated as acceptors on the charge transport property and device performance in non-fullerene (NF) bulk-heterojunction (BHJ) organic photovoltaic cells with a commercial polymer PTB7-Th as the donor material. Besides, the parent PDI molecule is studied as a control. Detailed charge carrier transport analysis is carried out on these PTB7-Th:Acceptor BHJs. Among all acceptor molecules, PTB7-Th:4PDI-ZnP film possesses the most desirable transport properties among the NF BHJs, and the best device performance with a power conversion efficiency (PCE) of 8.35%. To quantify the transport behaviors, the charge imbalance factor Δ is introduced to describe the global electron and hole balance in different electric fields. We discover that PTB7-Th:4PDI-ZnP has the least Δ and thereby gives rise to a BHJ cells with the highest fill factor and PCE.

For Zn-nanopapers obtained from grafting of Zn(II)-terpyridine complex (Zn-tpy) into tCNFs (2,2,6,6-tetramethylpiperidine-1-oxyl radical, TEMPO, oxidized cellulose nanofibrils), their optical hazes were first found to be highly dependent on alcohol-characteristic solvent stimulation. By addressing the controllable issue of benzyl alcohol (BA) disposal, the optical haze of Zn-nanopaper was adjusted to regulate from BA-induced instability wrinkling and swelling patterns, which was dictated by Zn-nanopaper thickness. Moreover, upon long-term UV radiation, these Zn-nanopapers exhibited stable UV-blocking, which, together with the optical haze adjustment, offered an opportunity for utilization in fluorescent lamps, flat panel displays or glass walls.

To address the intrinsic issue of conventional porphyrin derivatives with a deficient absorption between Soret and Q bands, we designed and synthesized two porphyrin molecules (BDTP-1 and BDTP-2) bearing a meso-alkyl substituted porphyrin core, benzodithiohene (BDT) ethynylene π-bridge and end-capping ethylrhodanine derivatives. Apart from the characteristic Soret and Q bands of porphyrin macrocycle, an extra peak (521 nm for BDTP-1 and 536 nm for BDTP-2) was derived from the BDT units. Using the porphyrin small molecules as electron donors and PC71BM as an electron acceptor, the devices show broad spectral photocurrent generation with a significant contribution from greenlight-harvesting (490–550 nm), resulting in high performances with PCEs up to 7.97%.

Fabricating multifunctional theranostic nanoparticles is highly pursued but still challenging for effective cancer treatment. Herein is reported a new theranostic nanoagent as both an MRI and targeted chemo/photothermal therapeutic agent. Prussian blue nanoparticles (PB) were first decorated with polydopamine (PDA), then conjugated with polyethylene glycol (PEG) and folic acid (FA), and finally loaded with doxorubicin (DOX) (denoted as PB@PDA@PEG-FA-DOX). The nanoagent was estimated to have an average size of 40 nm with a DOX-loading capacity of 36%, photothermal conversion efficiency of 45.7% and a transverse relaxation rate of 0.366 mM−1 s−1. In vitro release investigations showed a dual-responsive release by a mild acid and near-infrared (NIR) laser irradiation. PB@PDA@PEG-FA illustrated negligible cytotoxicity against the HL-7702 cell line and 38.2% cell viability under NIR against the HeLa cell line. PB@PDA@PEG-FA-DOX exhibited 45.2% cell viability. In contrast, the cell viability of PB@PDA@PEG-FA-DOX was dramatically decreased to 18.4% under NIR. Exclusive of folic acid, PB@PDA@PEG-DOX demonstrated 40.5% cell viability. These results demonstrated the potential of the nanoagent for integrated photothermal therapy (PTT) and chemotherapy, also embracing the FA targeting effect. In vivo MRI confirmed the effective nanoparticle accumulation, while infrared thermal images revealed the dramatically increased temperature under NIR at a tumor site. In vivo combination treatment-induced tumors were nearly completely destroyed without significant body weight loss after 14 days. H&E and Ki67 staining indicated remarkable necrosis and weak cell proliferation in the tumor area. Histologic examination revealed a lower toxicity in the vital organs. Therefore, this combination of chemo/photothermal therapy could provide an efficient route for cancer treatment.

Bis[di(4-methoxyphenyl)amino]carbazole-capped indacenodithiophenes (IDTs) have been constructed as hole transport materials (HTMs) for perovskite solar cells (PSCs). Two IDT-based HTMs, one with 3,6-bis[di(4-methoxyphenyl)amino]carbazole (YK1) and another with 2,7-bis[di(4-methoxyphenyl)amino]carbazole (YK2), show different performances in PSCs. The PSC device based on YK1 displays a very impressive PCE of 20.13% under AM1.5G solar illumination, which is much higher than those of the devices based on YK2 (17.35%) and Spiro-OMeTAD (19.01%) under the same working conditions. This is mainly because YK1 has more effective intermolecular π–π stacking, a lower-lying HOMO level and higher hole-mobility than YK2 and Spiro-OMeTAD. Furthermore, the YK1-based PSC exhibits excellent long-term stability retaining 94% of the initial PCE value after a 600 h lifetime without encapsulation owing to its better film morphology and hydrophobicity. These findings would shed light on the crucial importance of molecular engineering and allow its extension into general principles for the design of new HTMs for highly efficient and stable PSCs.