Isomerization Engineering of Oxygen-Enriched Carbon Quantum Dots for Efficient Electrochemical Hydrogen Peroxide Production.

Hydrogen peroxide (H2O2) has emerged as a kind of multi-functional green oxidants with extensive industrial utility. Oxidized carbon materials exhibit promises as electrocatalysts in the two-electron (2e-) oxygen reduction reaction (ORR) for H2O2 production. However, the precise identification and fabrication of active sites that selectively yield H2O2 present a serious challenge. Herein, a structural engineering strategy is employed to synthesize oxygen-doped carbon quantum dots (o-CQD) for the 2e- ORR. The surface electronic structure of the o-CQDs is systematically modulated by varying isomerization precursors, thereby demonstrating excellent electrocatalyst performance. Notably, o-CQD-3 emerges as the most promising candidate, showcasing a remarkable H2O2 selectivity of 96.2% (n = 2.07) at 0.68 V versus RHE, coupled with a low Tafel diagram of 66.95 mV dec-1. In the flow cell configuration, o-CQD-3 achieves a H2O2 productivity of 338.7 mmol gcatalyst -1 h-1, maintaining consistent production stability over an impressive 120-hour duration. Utilizing in situ technology and density functional theory calculations, it is unveil that edge sites of o-CQD-3 are facilely functionalized by C-O-C groups under alkaline ORR conditions. This isomerization engineering approach advances the forefront of sustainable catalysis and provides a profound insight into the carbon-based catalyst design for environmental-friendly chemical synthesis processes.

Elucidation of the synergistic effects of 3d metal (M = Cu, Co, and Ni) dopants and terminations (T = -O- and -OH) of Ti3C2Tx MXenes for urea adsorption ability via DFT calculations and experiments.

Dialysis is an artificial process to remove excess urea toxins from the body through adsorption or conversion. Urea adsorption by emergent 2D materials such as MXenes is one probable approach. Based on density functional theory (DFT) studies, the surface of Ti3C2Tx (T = -O- and -OH) MXenes is not optimum for urea adsorption. Therefore, functionalization with 3d metal dopants (Cu, Co, and Ni) is proposed to improve their urea adsorption ability. DFT calculations indicate that oxygen-terminated Ti3C2O2 has a much better urea adsorption ability when doped with Cu, Co, and Ni, with adsorption energy (Eads) values of -2.11 eV, -1.90 eV and -1.72 eV, respectively. These adsorption energies are much more favourable than that of the undoped one (Eads = -0.52 eV). To verify the calculation results, MILD Ti3C2Tx, or MXenes synthesized via the safer and easier minimally intensive layer delamination (MILD) method, were utilized to simulate Ti3C2O2 since they have -O- termination as the dominant species. Experimentally, the adsorption studies found that low concentration of Cu, Co, and Ni on MILD Ti3C2Tx showed a urea removal efficiency of 21.9%, 6.0% and 0.2%, respectively, much better than 0% removal efficiency of unfunctionalized Ti3C2Tx. Therefore, both DFT calculations and experiments showed that various metal functionalized MXenes have a similar trend for urea adsorption, highlighting the feasibility of using the computational approach to predict urea adsorption and further opening a new promising direction for the urea adsorption. Finally, this study is also the first to examine synergistic effects of metal dopants and surface terminations on MXenes for urea adsorption.

Flexible Wet-Spun PEDOT:PSS Microfibers Integrating Thermal-Sensing and Joule Heating Functions for Smart Textiles.

Multifunctional fiber materials play a key role in the field of smart textiles. Temperature sensing and active thermal management are two important functions of smart fabrics, but few studies have combined both functions in a single fiber material. In this work, we demonstrate a temperature-sensing and in situ heating functionalized conductive polymer microfiber by exploiting its high electrical conductivity and thermoelectric properties. The conductive polymer microfibers were prepared by wet-spinning the PEDOT:PSS aqueous dispersion with ionic liquid additives, which was used to enhance the electrical and mechanical properties of the final microfibers. The thermoelectric properties of these microfibers were further studied. Due to their excellent flexibility and mechanical properties, these fibers can be easily integrated into commercial fabrics for the manufacture of smart textiles through knitting. We further demonstrated a smart glove with integrated temperature-sensing and in situ heating functions, and further explored thermoelectric fiber-based temperature-sensing array fabric. These works combine the thermoelectric properties and heating function of conductive polymer fibers, providing new insights that enable further development of high-performance, multifunctional wearable smart textiles.

Thermostability enhancement of polyethylene terephthalate degrading PETase using self- and nonself-ligating protein scaffolding approaches.

Polyethylene terephthalate (PET) hydrolase enzymes show promise for enzymatic PET degradation and green recycling of single-use PET vessels representing a major source of global pollution. Their full potential can be unlocked with enzyme engineering to render activities on recalcitrant PET substrates commensurate with cost-effective recycling at scale. Thermostability is a highly desirable property in industrial enzymes, often imparting increased robustness and significantly reducing quantities required. To date, most engineered PET hydrolases show improved thermostability over their parental enzymes. Here, we report engineered thermostable variants of Ideonella sakaiensis PET hydrolase enzyme (IsPETase) developed using two scaffolding strategies. The first employed SpyCatcher-SpyTag technology to covalently cyclize IsPETase, resulting in increased thermostability that was concomitant with reduced turnover of PET substrates compared to native IsPETase. The second approach using a GFP-nanobody fusion protein (vGFP) as a scaffold yielded a construct with a melting temperature of 80°C. This was further increased to 85°C when a thermostable PETase variant (FAST PETase) was scaffolded into vGFP, the highest reported so far for an engineered PET hydrolase derived from IsPETase. Thermostability enhancement using the vGFP scaffold did not compromise activity on PET compared to IsPETase. These contrasting results highlight potential topological and dynamic constraints imposed by scaffold choice as determinants of enzyme activity.

Unveiling Charge-Transfer Dynamics at Singlet Fission Layer/Hybrid Perovskite Interface.

Singlet fission (SF) materials have been applied in various types of solar cells to pursue higher power conversion efficiency (PCE) beyond the Shockley-Queisser (SQ) limit. SF implementation in perovskite solar cells has not been successfully realized yet due to the insufficient understanding of the SF/perovskite heterojunctions. In this work, we attempt to elucidate the charge dynamics of an SF/perovskite system by incorporating a well-known SF molecule, TIPS-pentacene, and a triple-cation perovskite Cs0.05(FA0.85MA0.15)0.95PbI2.55Br0.45, owing to their well-matched energy structures. The transient absorption spectra and kinetic fitting plots suggest an electron-transfer process from the triplet state of TIPS-pentacene to perovskite in the picosecond regime, which increases the carrier density by 20% in the perovskite layer. This work confirms the existence of an electron-transfer process between the SF material and perovskite, providing a pathway to SF-enhanced perovskite solar cells.

High-Performance Semi-Transparent Perovskite Solar Cells with over 22% Visible Transparency: Pushing the Limit through MXene Interface Engineering.

Semi-transparent perovskite solar cells (ST-PSCs) have attracted enormous attention recently due to their potential in building-integrated photovoltaic. To obtain adequate average visible transmittance (AVT), a thin perovskite is commonly employed in ST-PSCs. While the thinner perovskite layer has higher transparency, its light absorption efficiency is reduced, and the device shows lower power conversion efficiency (PCE). In this work, a combination of high-quality transparent conducting layers and surface engineering using 2D-MXene results in a superior PCE. In situ high-temperature X-ray diffraction provides direct evidence that the MXene interlayer retards the perovskite crystallization process and leads to larger perovskite grains with fewer grain boundaries, which are favorable for carrier transport. The interfacial carrier recombination is decreased due to fewer defects in the perovskite. Consequently, the current density of the devices with MXene increased significantly. Also, optimized indium tin oxide provides appreciable transparency and conductivity as the top electrode. The semi-transparent device with a PCE of 14.78% and AVT of over 26.7% (400-800 nm) was successfully obtained, outperforming most reported ST-PSCs. The unencapsulated device maintained 85.58% of its original efficiency after over 1000 h under ambient conditions. This work provides a new strategy to prepare high-efficiency ST-PSCs with remarkable AVT and extended stability.

Effect of Air Exposure on Electron-Beam-Induced Degradation of Perovskite Films.

Organic-inorganic halide perovskites are interesting candidates for solar cell and optoelectronic applications owing to their advantageous properties such as a tunable band gap, low material cost, and high charge carrier mobilities. Despite making significant progress, concerns about material stability continue to impede the commercialization of perovskite-based technology. In this article, we investigate the impact of environmental parameters on the alteration of structural properties of MAPbI3 (CH3NH3PbI3) thin films using microscopy techniques. These characterizations are performed on MAPbI3 thin films exposed to air, nitrogen, and vacuum environments, the latter being possible by using dedicated air-free transfer setups, after their fabrication into a nitrogen-filled glovebox. We observed that even less than 3 min of air exposure increases the sensitivity to electron beam deterioration and modifies the structural transformation pathway as compared to MAPbI3 thin films which are not exposed to air. Similarly, the time evolution of the optical responses and the defect formation of both air-exposed and non-air-exposed MAPbI3 thin films are measured by time-resolved photoluminescence. The formation of defects in the air-exposed MAPbI3 thin films is first observed by optical techniques at longer timescales, while structural modifications are observed by transmission electron microscopy (TEM) measurements and supported by X-ray photoelectron spectroscopy (XPS) measurements. Based on the complementarity of TEM, XPS, and time-resolved optical measurements, we propose two different degradation mechanism pathways for air-exposed and non-air-exposed MAPbI3 thin films. We find that when exposed to air, the crystalline structure of MAPbI3 shows gradual evolution from its initial tetragonal MAPbI3 structure to PbI2 through three different stages. No significant structural changes over time from the initial structure are observed for the MAPbI3 thin films which are not exposed to air.

Oxide-Derived Bismuth as an Efficient Catalyst for Electrochemical Reduction of Flue Gas.

Post-combustion flue gas (mainly containing 5-40% CO2 balanced by N2 ) accounts for about 60% global CO2 emission. Rational conversion of flue gas into value-added chemicals is still a formidable challenge. Herein, this work reports a ß-Bi2 O3 -derived bismuth (OD-Bi) catalyst with surface coordinated oxygen for efficient electroreduction of pure CO2 , N2, and flue gas. During pure CO2 electroreduction, the maximum Faradaic efficiency (FE) of formate reaches 98.0% and stays above 90% in a broad potential of 600 mV with a long-term stability of 50 h. Additionally, OD-Bi achieves an ammonia (NH3 ) FE of 18.53% and yield rate of 11.5 µg h-1 mgcat -1 in pure N2 atmosphere. Noticeably, in simulated flue gas (15% CO2 balanced by N2 with trace impurities), a maximum formate FE of 97.3% is delivered within a flow cell, meanwhile above 90% formate FEs are obtained in a wide potential range of 700 mV. In-situ Raman combined with theory calculations reveals that the surface coordinated oxygen species in OD-Bi can drastically activate CO2 and N2 molecules by selectively favors the adsorption of *OCHO and *NNH intermediates, respectively. This work provides a surface oxygen modulation strategy to develop efficient bismuth-based electrocatalysts for directly reducing commercially relevant flue gas into valuable chemicals.

One-Pot Synthesis of Aminated Bimodal Mesoporous Silica Nanoparticles as Silver-Embedded Antibacterial Nanocarriers and CO2 Capture Sorbents.

Mesoporous silica nanoparticles have highly versatile structural properties that are suitable for a plethora of applications including catalysis, separation, and nanotherapeutics. We report a one-pot synthesis strategy that generates bimodal mesoporous silica nanoparticles via coassembly of a structure-directing Gemini surfactant (C16-3-16) with a tetraethoxysilane/(3-aminopropyl)triethoxysilane-derived sol additive. Synthesis temperature enables control of the nanoparticle shape, structure, and mesopore architecture. Variations of the aminosilane/alkylsilane molar ratio further enable programmable adjustments of hollow to core-shell and dense nanoparticle morphologies, bimodal pore sizes, and surface chemistries. The resulting Gemini-directed aminated mesoporous silica nanoparticles have excellent carbon dioxide adsorption capacities and antimicrobial properties against Escherichia coli. Our results provide an enhanced understanding of the structure formation of multiscale mesoporous inorganic materials that are desirable for numerous applications such as carbon sequestration, water remediation, and biomedical-related applications.

Phosphorus-Doped Graphene Aerogel as Self-Supported Electrocatalyst for CO2 -to-Ethanol Conversion.

Electrochemical reduction of carbon dioxide (CO2 ) to ethanol is a promising strategy for global warming mitigation and resource utilization. However, due to the intricacy of C─C coupling and multiple proton-electron transfers, CO2 -to-ethanol conversion remains a great challenge with low activity and selectivity. Herein, it is reported a P-doped graphene aerogel as a self-supporting electrocatalyst for CO2 reduction to ethanol. High ethanol Faradaic efficiency (FE) of 48.7% and long stability of 70 h are achieved at -0.8 VRHE . Meanwhile, an outstanding ethanol yield of 14.62 µmol h-1 cm-2 can be obtained, outperforming most reported electrocatalysts. In situ Raman spectra indicate the important role of adsorbed *CO intermediates in CO2 -to-ethanol conversion. Furthermore, the possible active sites and optimal pathway for ethanol formation are revealed by density functional theory calculations. The graphene zigzag edges with P doping enhance the adsorption of *CO intermediate and increase the coverage of *CO on the catalyst surface, which facilitates the *CO dimerization and boosts the EtOH formation. In addition, the hierarchical pore structure of P-doped graphene aerogels exposes abundant active sites and facilitates mass/charge transfer. This work provides inventive insight into designing metal-free catalysts for liquid products from CO2 electroreduction.

Novel Materials for Urban Farming.

Scarcity of natural resources, shifting demographics, climate change, and increasing waste are four major challenges in the quest to feed the exploding world population. These challenges serve as the impetus to harness novel technologies to improve agriculture, productivity, and sustainability. Urban farming has several advantages over conventional farming: higher productivity, improved sustainability, and the ability to provide fresh food all year round. Novel materials are key to accelerating the evolution of urban farming - with their ability to facilitate controlled release of nutrients and pesticides, improved seed health, substrates with better water retention capability, more efficient recycling of agricultural waste, and precise plant health monitoring. Materials science enables environmental sustainability and higher harvest yields in urban farms. Here, Singapore is used as an example of a land-scarce city where urban farming may be the solution for future food production. Potential research directions and challenges in urban farming are highlighted, and how material optimization and innovation drive the development of urban farming to meet national and global food demands is briefly discussed. This review serves as a guide for researchers and a reference for stakeholders of urban farms, policy makers, and other interested parties.

Assessment of heavy metal and metalloid levels and screening potential of tropical plant species for phytoremediation in Singapore.

Heavy metal or metalloid contamination is a common problem in soils of urban environments. Their introduction can be due to unpremeditated anthropogenic activities like atmospheric deposition produced by diffuse sources, construction activities and landscape maintenance. Phytoremediation is a rapidly evolving, sustainable approach to remediate the contaminated lands where metals and metalloids are highly persistent in the environment. The present work sets out to determine the level of 12 heavy metals and metalloids (As, Cd, Co, Cr, Cu, Fe, Mn, Mo, Ni, Pb, Sb and Zn) in soil and their accumulation by plant foliage found in nature parks and industrial sites in Singapore. The latter also involve the investigation of the remediation capacity of selected tropical plant species found at the sampling sites. The study is done using digestion and inductively coupled plasma-optical emission spectrometry. Eleven soil sampling sites across Singapore with 300 sampling points were selected, where soil (0-10 cm) and plant foliage samples were collected. Bioconcentration factors were determined to assess the phytoremediation potential of the collected plant species. Toxicity risk of heavy metals were assessed by comparing the target and intervention values from the soil quality guidelines by the Dutch Standard. Results of the study revealed there were regions where levels of heavy metals and metalloids were relatively high and could affect the environment and the health of flora and fauna in Singapore. Our study discovered that there were available tropical plant species (e.g., wildflowers, ferns and shrubs) which could potentially play a significant role in the remediation of contaminated lands that could open up a huge possibility of developing a sustainable and environmentally-friendly way of managing this emerging urban problem. Results showed that 12 plant species, including hyperaccumulator like Pteris vittata, Centella asiatica, were effective for the accumulation of heavy metals and metalloids.

Double-Chain Cationic Surfactants: Swelling, Structure, Phase Transitions and Additive Effects.

Double-chain amphiphilic compounds, including surfactants and lipids, have broad significance in applications like personal care and biology. A study on the phase structures and their transitions focusing on dioctadecyldimethylammonium chloride (DODAC), used inter alia in hair conditioners, is presented. The phase behaviour is dominated by two bilayer lamellar phases, Lß and Lα, with "solid" and "melted" alkyl chains, respectively. In particular, the study is focused on the effect of additives of different polarity on the phase transitions and structures. The main techniques used for investigation were differential scanning calorimetry (DSC) and small- and wide-angle X-ray scattering (SAXS and WAXS). From the WAXS reflections, the distance between the alkyl chains in the bilayers was obtained, and from SAXS, the thicknesses of the surfactant and water layers. The Lα phase was found to have a bilayer structure, generally found for most surfactants; a Lß phase made up of bilayers with considerable chain tilting and interdigitation was also identified. Depending mainly on the polarity of the additives, their effects on the phase stabilities and structure vary. Compounds like urea have no significant effect, while fatty acids and fatty alcohols have significant effects, but which are quite different depending on the nonpolar part. In most cases, Lß and Lα phases exist over wide composition ranges; certain additives induce transitions to other phases, which include cubic, reversed hexagonal liquid crystals and bicontinuous liquid phases. For a system containing additives, which induce a significant lowering of the Lß-Lα transition, we identified the possibility of a triggered phase transition via dilution with water.

Pressure-Responsive Two-Dimensional Metal-Organic Framework Composite Membranes for CO2 Separation.

The regulation of permeance and selectivity in membrane systems may allow effective relief of conventional energy-intensive separations. Here, pressure-responsive ultrathin membranes (≈100 nm) fabricated by compositing flexible two-dimensional metal-organic framework nanosheets (MONs) with graphene oxide nanosheets for CO2 separation are reported. By controlling the gas permeation direction to leverage the pressure-responsive phase transition of the MONs, CO2 -induced gate opening and closing behaviors are observed in the resultant membranes, which are accompanied with the sharp increase of CO2 permeance (from 173.8 to 1144 gas permeation units) as well as CO2 /N2 and CO2 /CH4 selectivities (from 4.1 to 22.8 and from 4 to 19.6, respectively). The flexible behaviors and separation mechanism are further elucidated by molecular dynamics simulations. This work establishes the relevance of structural transformation-based framework dynamics chemistry in smart membrane systems.

Two Birds with One Stone: FeS2@C Yolk-Shell Composite for High-Performance Sodium-Ion Energy Storage and Electromagnetic Wave Absorption.

Cost-effective material with a rational design is significant for both sodium-ion batteries (SIBs) and electromagnetic wave (EMW) absorption. Herein, we report an elaborate yolk-shell FeS2@C nanocomposite as a promising material for application in both SIBs and EMW absorption. When applied as an anode material in SIBs, the yolk-shell structure not only facilitates a fast electron transport and shortens Na ion diffusion paths but also eases the huge volume change of FeS2 during repeated discharge/charge processes. The as-developed FeS2@C exhibits a high specific capacity of 616 mA h g-1 after 100 cycles at 0.1 A g-1 with excellent rate performance. Furthermore, owing to the significant cavity and interfacial effects enabled by yolk-shell structuring, the FeS2@C nanocomposite delivers excellent EMW absorption properties with a strong reflection loss (-45 dB with 1.45 mm matching thickness) and a broad 15.4 GHz bandwidth. This work inspires the development of high-performance bifunctional materials.

Facile control of surfactant lamellar phase transition and adsorption behavior.

This study sets out to investigate the effect of the presence of small water-soluble additives on the tunability of the surfactant gel-to-liquid crystalline (Lß-Lα) phase transition temperature (T m) for a bilayer-forming cationic surfactant and the phase behavior of such surfactant systems on dilution. This is strongly driven by the fact that this type of cationic surfactant has many interesting unanswered scientific questions and has found applications in various areas such as consumer care, the petrochemical industry, food science, etc. The underlying surfactant/additive interactions and the interfacial behavior of lamellar surfactant systems including the surfactant deposition on surfaces can provide new avenues to develop novel product formulations. We have examined dioctadecyldimethyl ammonium chloride (DODAC) in the presence of small polar additives, with respect to the phase behavior upon dilution and the deposition on silica. Differential scanning calorimetry (DSC) is used to track the transition temperature, T m, and synchrotron and laboratory-based small and wide-angle X-ray scattering (SAXS and WAXS) were used to determine the self-assembled surfactant structure below and above the T m. DSC scans showed that upon dilution the additives could be removed from the surfactant bilayer which in turn tuned the T m. A spontaneous transition from a liquid crystalline (Lα) phase to a gel (Lß) phase on dilution was demonstrated, which indicated that additives could be taken out from the Lα phase. By means of in situ null ellipsometry, the deposition of a diluted surfactant Lß phase upon replacement of bulk solution by deionized water was followed. This technique enables time-resolved monitoring of the deposited surfactant layer thickness and adsorbed amount, which allows us to understand the deposition on surfaces. Robust layers at least one bilayer-thick were deposited onto the surface and shown to be irreversibly adsorbed due to poor surfactant solvency in water. The thickest layer of surfactant deposited after dilution was found for mixtures with small amounts of additive since high amounts might lead to a phase-separated system.

Molecular Aggregation of Naphthalene Diimide(NDI) Derivatives in Electron Transport Layers of Inverted Perovskite Solar Cells and Their Influence on the Device Performance.

One of key factors to design applicable electron transport layers (ETLs) for perovskite solar cells is the morphology of ETLs since a good morphology would help to facilitate the carrier transport at two interfaces (perovskite\ETL and ETL\cathode). However, one drawback of most organic ETL small molecules is the internal undesired accumulation, which would cause the formation of inappropriate morphology and rough ETL surface. Here, by elaborately designing the side chains of NDI derivatives, the molecular interaction could be modified to achieve the aggregation in different degrees, which would eventually affect the accumulation of molecules and surface qualities of ETLs. By speculating from the comparison between the absorption spectra of solutions and films, the sequence of extent of molecule interaction and aggregation was built among three NDI derivatives, which is further confirmed by direct evidence of atomic force microscopy (AFM) images. Then, carrier exaction abilities are simply studied by steady-state photoluminescence spectroscopy. The carrier transport process is also discussed based on cyclic voltammetry, time-resolved photoluminescence spectroscopy and mobility. NDIF1 are proven to have the appropriate internal aggregation to smooth the contact with cathode and low series resistance, and a device performance of 15.6 % is achieved. With the ability of preventing the thermal diffusion of Ag towards the perovskite surface due to the strong interaction between molecules, NDIF2 at high concentration shows the highest fill factor (80 %).

Monitoring Electron-Phonon Interactions in Lead Halide Perovskites Using Time-Resolved THz Spectroscopy.

Lead halide perovskite semiconductors have low-frequency phonon modes within the lead halide sublattice and thus are considered to be soft. The soft lattice is considered to be important in defining their interesting optoelectronic properties. Electron-phonon coupling governs hot-carrier relaxation, carrier mobilities, carrier lifetimes, among other important electronic characteristics. Directly observing the interplay between free charge carriers and phonons can provide details on how phonons impact these properties (e.g., exciton populations and other collective modes). Here, we observe a delicate interplay among carriers, phonons, and excitons in mixed-cation and mixed-halide perovskite films by simultaneously resolving the contribution of charge carriers and phonons in time-resolved terahertz photoconductivity spectra. We are able to observe directly the increase in phonon population during carrier cooling and discuss how thermal equilibrium populations of carriers and phonons modulate the carrier transport properties, as well as reduce the population of carriers within band tails. We are also able to observe directly the formation of free charge carriers when excitons interact with phonons and dissociate and to describe how free carriers and exciton populations exchange through phonon interactions. Finally, we also time-resolve how the carriers are screened via the Coulomb interaction at low and room temperatures. Our studies shed light on how charge carriers interact with the low-energy phonons and discuss implications.

Multiscale Self-Assembly of a Phenyl-Flanked Diketopyrrolopyrrole Derivative: A Solution-Processable Building Block for π-Conjugated Supramolecular Polymers.

We report a solution-processable π-conjugated molecular building block (denoted as PhDPP) consisting of a rigid and planar core of phenyl-flanked diketopyrrolopyrrole and "soft" branched alkoxy chains that endow the solubility in a variety of organic solvents. Intermolecular hydrogen bonding in PhDPP was revealed in nonpolar solvents above a threshold of concentration and below a critical point of temperature. The strong intermolecular interaction mainly contributed by the hydrogen-bonding and π-π interaction between PhDPP molecules promoted the formation of supramolecular polymeric structures in both solution and solid states and at interfaces. The supramolecular polymeric properties enabled solution-based processing of PhDPP under a variety of conditions into different structures including fibers and uniform thin films. The structure-property relationship that we established in the present system of PhDPP from the molecular to supramolecular level will be important to solution-process this type of H-bonding π-conjugated molecules for a variety of applications such as optoelectronic devices.