As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and “earth-abundant” nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C3N4 and g-C3N4-based nanocomposites, including (1) nanoarchitecture design of bare g-C3N4, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C3N4 at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C3N4 with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The constructi...

Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

We fabricated a perovskite solar cell that uses a double layer of mesoporous TiO2 and ZrO2 as a scaffold infiltrated with perovskite and does not require a hole-conducting layer. The perovskite was produced by drop-casting a solution of PbI2, methylammonium (MA) iodide, and 5-ammoniumvaleric acid (5-AVA) iodide through a porous carbon film. The 5-AVA templating created mixed-cation perovskite (5-AVA)x(MA)1- xPbI3 crystals with lower defect concentration and better pore filling as well as more complete contact with the TiO2 scaffold, resulting in a longer exciton lifetime and a higher quantum yield for photoinduced charge separation as compared to MAPbI3. The cell achieved a certified power conversion efficiency of 12.8% and was stable for >1000 hours in ambient air under full sunlight.

https://science.sciencemag.org/content/sci/345/6194/295.full.pdf

A hole-conductor-free, fully printable mesoscopic perovskite solar cell with high stability

The photovoltaics of organic–inorganic lead halide perovskite materials have shown rapid improvements in solar cell performance, surpassing the top efficiency of semiconductor compounds such as CdTe and CIGS (copper indium gallium selenide) used in solar cells in just about a decade. Perovskite preparation via simple and inexpensive solution processes demonstrates the immense potential of this thin-film solar cell technology to become a low-cost alternative to the presently commercially available photovoltaic technologies. Significant developments in almost all aspects of perovskite solar cells and discoveries of some fascinating properties of such hybrid perovskites have been made recently. This Review describes the fundamentals, recent research progress, present status, and our views on future prospects of perovskite-based photovoltaics, with discussions focused on strategies to improve both intrinsic and extrinsic (environmental) stabilities of high-efficiency devices. Strategies and challenges regardi...

Halide Perovskite Photovoltaics: Background, Status, and Future Prospects

In recent years, the record efficiency of perovskite solar cells (PSCs) has been updated from 9.7% to 20.1%. However, there has been very little study of the issue of stability, which restricts the outdoor application of PSCs. The issues of the degradation of perovskite and the stability of PSC devices should be urgently addressed to achieve good reproducibility and long lifetimes for PSCs with high conversion efficiency. Without studies on stability, exciting achievements cannot be transferred from the laboratory to industry and outdoor applications. In order to improve their stability, a basic understanding of the degradation process of PSCs in different conditions should be acquired via thorough study. This review summarizes recent studies of the relationship of the chemical stability of PSCs with their environment (oxygen and moisture, UV light, solution process, temperature) and corresponding possible solutions.

Review of recent progress in chemical stability of perovskite solar cells

The appropriate interfacial contact of heterojunction photocatalysts plays a critical role in transfer/separation of interfacial charge carriers. Design of two-dimensional (2D)/2D surface-to-surface heterojunction is an effective method for improving photocatalytic activity since greater contact area can enhance interfacial charge transfer rate. Herein, ultrathin 2D/2D WO3/g-C3N4 step-like composite heterojunction photocatalysts were fabricated by electrostatic self-assembly of ultrathin tungsten trioxide (WO3) and graphitic carbon nitride (g-C3N4) nanosheets. The ultrathin WO3 and g-C3N4 nanosheets were obtained by electrostatic-assisted ultrasonic exfoliation of bulk WO3 and a two-step thermal-etching of bulk g-C3N4, respectively. The thickness of ultrathin WO3 and g-C3N4 nanosheets are 2.5–3.5 nm, which is equivalent to 5–8 atomic or molecular layer thickness. This ultrathin layered heterojunction structure can enhance surface photocatalytic rate because photogenerated electrons and holes at heterogeneous interface more easily transfer to surface of photocatalysts. Therefore, the obtained ultrathin 2D/2D WO3/g-C3N4 step-scheme (S-scheme) heterojunction photocatalysts exhibited better H2-production activity than pure g-C3N4 and WO3 with the same loading amount of Pt as cocatalyst. The mechanism and driving force of charge transfer and separation in S-scheme heterojunction photocatalysts are investigated and discussed. This investigation will provide new insight about designing and constructing novel S-scheme heterojunction photocatalysts.

Ultrathin 2D/2D WO3/g-C3N4 step-scheme H2-production photocatalyst

Efficient hole-conductor-free organic lead iodide thin film solar cells have been fabricated with a sequential deposition method, and a highest efficiency of 10.49% has been achieved. Meanwhile, the ideal current-voltage model for a single heterojunction solar cell is applied to clarify the junction property of the cell. The model confirms that the TiO2/CH3NH3PbI3/Au cell is a typical heterojunction cell and the intrinsic parameters of the cell are comparable to that of the high-efficiency thin-film solar cells.

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Hole-conductor-free perovskite organic lead iodide heterojunction thin-film solar cells: High efficiency and junction property

From Ultrafast to Ultraslow: Charge-Carrier Dynamics of Perovskite Solar Cells

An all-carbon counter electrode has been fabricated for hole-conductor-free organo-metal perovskite heterojunction thin-film solar cells by a simple and low-temperature process. The counter electrode consisted of two parts: a mesoscopic carbon layer for good contact with the perovskite layer, and a piece of industrial flexible graphite sheet as the conducting electrode. Several types of carbon materials were employed in the counter electrodes and tested. From an electrochemical impedance study, it is found that the contact between the counter electrode and perovskite layer has a significant influence on the charge transport properties of the cells. A power conversion efficiency up to 10.2% has been achieved by hole-conductor-free mesoscopic CH3NH3PbI3/TiO2 heterojunction solar cells with the counter electrode containing a composition of graphite and carbon black, which inspires a new promising route towards low-cost and large-scale commercialization of perovskite solar cells.

An all-carbon counter electrode for highly efficient hole-conductor-free organo-metal perovskite solar cells

Hybrid organic–inorganic perovskites (e.g., CH3NH3PbI3) are promising light absorbers for the third-generation photovoltaics. Herein we demonstrate a modified two-step deposition method to fabricate a uniform CH3NH3PbI3 capping layer with high-coverage and thickness of 300 nm on top of the mesoporous TiO2. The CH3NH3PbI3 layer shows high light-harvesting efficiency and long carrier lifetime over 50 ns. On the basis of the as-prepared film, TiO2/CH3NH3PbI3 heterojunction solar cells achieve a power conversion efficiency of 10.47% with a high open-circuit voltage of 948 mV, the highest recorded to date for hole-transport-material-free (HTM-free) perovskite-based heterojunction cells. The efficiency exceeding 10% shows promising prospects for the HTM-free solar cells based on organic lead halides.

Huijue Wu

Papers

Hole-conductor-free perovskite organic lead iodide heterojunction thin-film solar cells: High efficiency and junction property

From Ultrafast to Ultraslow: Charge-Carrier Dynamics of Perovskite Solar Cells

An all-carbon counter electrode for highly efficient hole-conductor-free organo-metal perovskite solar cells

Modified Two-Step Deposition Method for High-Efficiency TiO2/CH3NH3PbI3 Heterojunction Solar Cells

Self‐Adhesive Macroporous Carbon Electrodes for Efficient and Stable Perovskite Solar Cells