CO2 hydrogenation to light olefins is regarded as a promising route for carbon utilization and sustainable chemical production. Nevertheless, the development of efficient catalysts remains challenging because it is difficult to simultaneously enhance CO2 activation, C-C coupling, and CH4 suppression, largely due to insufficient interfacial synergy among active components and inadequate support regulation. In this work, Cu-Ni-Ce/SiO2-CaO multicomponent catalysts with different Cu/Ni ratios were synthesized via coprecipitation and evaluated for selective CO2 hydrogenation to light olefins. BET, XRD, XPS, and SEM results revealed highly dispersed multimetallic active species and mesoporous structures, while CaO incorporation enhanced CO2 adsorption, strengthened metal-support interaction, and inhibited particle agglomeration. Among the prepared catalysts, 2Cu1Ni1Ce/SiO2-CaO exhibited the most favorable textural properties and the best catalytic performance among the tested Cu/Ni ratios, affording a CO2 conversion of approximately 15.00% and a C2-C3 selectivity of 76.69% with suppressed CH4 formation. Further optimization of the reaction conditions showed that increasing the H2/CO2 ratio from 1:1 to 3:1 improved the CO2 conversion from 7.21% to 15.14%, while raising the reaction pressure from 1 to 4 MPa further increased the CO2 conversion from 6% to 18% and enhanced the light olefin selectivity to approximately 80%. XPS results suggested that Ni0 sites promoted CO2 activation and CO formation, whereas adjacent Cu+/Cu0 sites facilitated subsequent hydrogenation and C-C coupling. Overall, these results demonstrate that rational construction of Cu-Ni-Ce interfacial synergy, together with SiO2-CaO support engineering, is an effective strategy for improving light olefin production from CO2 hydrogenation.
Two-dimensional transition-metal dichalcogenides (TMDs) are commonly used in catalytic reactions due to their inexpensive and easy-to-prepare nature, but the monolithic structure limits their applicability to overall water splitting. In this work, for the first time, we introduce single-atom Cr doping at the interface of a MoS2/1T-WS2 heterojunction, achieving a synergistic reconstruction of the interfacial electronic structure and the built-in electric field, thereby simultaneously activating the key steps of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). In 1 M KOH, Cr@MoS2/WS2 requires only 145 mV (HER) and 181 mV (OER) at 10 mA cm- 2, and it remains stable during continuous operation for 72 h at 100 mA cm-2. Spectroscopy and density functional theory (DFT) jointly reveal enhanced Cr-S coordination and d/p-orbital hybridization, along with regulation of the band gap and band-center, establishing a generalizable paradigm from interfacial doping to electronic reconstruction and ultimately to performance improvement. This interfacial doping strategy can be generalized for multifunctional catalytic modification of other transition metal disulfides.
Crystalline silicon solar cells have long dominated the global photovoltaic market due to their mature manufacturing processes, excellent stability, and abundant raw material reserves, accounting for over 90% of the total PV market share. However, single−junction c−Si solar cells are approaching the Shockley–Queisser (SQ) efficiency limit of ~29.4%, creating an urgent need for next−generation PV technologies to achieve higher power conversion efficiency (PCE). Monolithic perovskite/silicon tandem solar cells (PSTSCs) stand as the most commercially promising technology to surpass the single−junction efficiency limit. Since their first demonstration in 2015, PSTSCs have experienced rapid technological advancement, with the certified PCE reaching 35.0% in 2026. This review posits that their rapid efficiency ascent is not serendipitous but driven by synergistic innovations across critical subsystems. We systematically deconstruct these efficiency drivers, encompassing top−cell materials, bottom−cell architecture, and optical management. We conclude by outlining future research frontiers essential for transforming this lab−champion technology into a mainstream energy solution.
III-V colloidal quantum dots (CQDs) with large and well-controlled diameters are of interest in applications from red light emitters to deep short-wave infrared (SWIR) photodetectors, yet nanocluster-seeded syntheses often encounter an empirical "size wall" in the ∼5-8 nm diameter range. Here, we identify monomer release and transfer from nanoclusters to growing seeds as a key kinetic constraint during extended injection and growth. We show that short-chain carboxylic acids (SCCAs) can act as transient ligands that increase nanocluster lability and enhance monomer transfer, enabling continuous growth beyond this plateau. 1H NMR using 13C-labeled acetic acid quantifies a ∼1:1 myristate/acetate ligand ratio on the initial nanoclusters, with diffusion-ordered spectroscopy (DOSY) supporting the transient surface association of acetate; 2H NMR of CQDs grown with deuterated acetic acid (CD3COOH) shows no residual deuterium signal, indicating that acetate promotes growth without persisting on the final CQD surface. Across a C1 (formic) to C4 (butyric) SCCA screen, C2 (acetic) acid provides the best balance of volatility and lability. Incorporating SCCAs at the nanocluster stage yields InAs CQDs with excitonic features extending up to 1800 nm. XPS and indium K-edge XANES/EXAFS analyses indicate diminished oxide-related features in acetic acid-derived samples compared with size-matched controls. We fabricate photodetectors with a 1520 nm exciton, extending InAs CQD photodetection into the deep SWIR.
Realizing multilayer stacks analogous to classical semiconductors with precise control over chemistry, composition, thickness, orientation, and epitaxy using solution-processing has remained a long-standing bottleneck. Here, we present a novel scalable solution-based strategy for the deterministic deposition of any perovskite layer onto an existing perovskite film, enabling multilayer perovskite heterostructures with comparable control. Our approach dissolves pre-synthesized perovskite crystals or precursor salts in a dissolving solvent, followed by dispersion into a miscible carrier solvent to form a metastable colloidal system that can be deposited without disturbing the underlying layer. This universal process enables architectures including 3D-on-3D, 2D|3D, 3D|2D, and more complex multilayers, while independently controlling composition, thickness, orientation, and interfaces. We further show that lattice parameter matching enables orientation control through solution-phase epitaxy. Integrating a formamidinium-rich 3D|2D stack (FA 0.9 Cs 0.1 PbI 3 |(3AMP)FA 2 Pb 3 I 10 ) into p-i-n solar cells increases efficiency from 24.2% to 26.0%, maintained for 2D layer thicknesses up to 80 nm, establishing a versatile platform for scalable semiconductor heterostructures.
High crystallographic symmetry is a key feature of many inorganic semiconductors and underpins their remarkable physical properties. By contrast, hybrid (organic and inorganic) crystals such as two-dimensional metal halide perovskites exhibit much lower crystal symmetry due to in-plane or out-of-plane octahedral distortions. Although they exhibit efficient photoinduced emission at room temperature, limited control over charge carrier transport remains a major challenge for optoelectronic applications. Here, inspired by three-dimensional cubic (alpha-phase) FAPbI3 (FA, formamidinium), we developed FA-based layered two-dimensional perovskites using tailored cage cations, spacers and crystallization protocols. The compounds achieve near-maximal predicted symmetry, adopting a tetragonal P4/mmm space group without octahedral distortion. Among reported two-dimensional perovskites, these materials present short interlayer distances (4 & Aring;) and lower optical bandgaps (1.7-1.8 eV). The absence of octahedral distortions results in an exciton diffusion length of 2.5 & micro;m and a diffusivity of 4.4 cm2 s-1, both of which are an order of magnitude larger than those of previously reported two-dimensional perovskites and are on par with monolayer transition metal dichalcogenides.
Metal halide perovskites degrade under the same illumination that powers them, yet nanoscale observation of this photochemistry is confounded by electron-beam damage in transmission electron microscopy (TEM). We introduce an optical-fiber-coupled closed-cell TEM platform with independent control over electron dose rate, illumination wavelength and power density, and gas environment, and use it to decouple photochemical from radiolytic degradation in CsPbBr3 in real time. After establishing beam-safe imaging conditions, we find that above-bandgap illumination induces preferential emergence of PbBr2 domains, the dominant detectable crystalline product, primarily at grain boundaries. In contrast, the electron beam alone reduces Pb2+ to metallic Pb0, a chemically and spatially distinct pathway. Sub-bandgap illumination produces no detectable spectroscopic change, supporting photocarrier generation rather than optical power deposition as a dominant driver. Decoupling light from the electron beam is a prerequisite for real-time imaging photochemistry in beam-sensitive materials.
Perovskite-silicon triple-junction photovoltaics offer efficiency gains beyond dual-junction devices but at the expense of added complexity1. Here we address two key bottlenecks in perovskite-silicon-based triple-junction solar cells: reduced open-circuit voltage (VOC) in the wide-bandgap (WBG) top cell and limited photocurrent generation in the middle cell1,2. A non-volatile additive, 4-hydroxybenzylamine (HBA), regulates WBG perovskite crystallization and passivates defects, promoting oriented growth and suppressing non-radiative recombination. Together with improved energy-level alignment, this yields VOCs of up to 1.405 V and enhanced stability. To overcome the current limitations in the middle cell, a three-step deposition strategy enables the formation of thick, low-bandgap perovskite absorbers while preserving microstructural integrity and enhancing electron extraction. Also, low-refractive-index SiOx-nanoparticles (SiOx-np) that accumulate in the front valleys of the textured silicon bottom cell act as an optical middle reflector, enhancing light absorption in the middle cell. These advances are then combined in 1-cm2 perovskite-perovskite-silicon devices, achieving a certified efficiency of 30.02%.
CO2 electroreduction (CO2E) uses electricity to produce valuable chemicals and fuels. Although much fundamental progress has been made, industrial adoption will rely on an appropriate combination of CO2E energy efficiency, capital cost and lifetime, as well as electricity and carbon price, to achieve a competitive levelized cost of chemicals/fuels. Here we discuss how a consistent set of testing conditions, third-party accreditation and intersectoral partnerships can prepare CO2E for its transition from bench-scale prototypes to industrial deployment. Drawing on lessons from photovoltaics—which progressed from the laboratory to globally deployed product once the levelized cost of electricity reached grid parity—we recommend establishing robust, transparent testing procedures, as well as objective certification frameworks. We also discuss disanalogies to photovoltaics—how standardizing CO2E feedstocks, product analysis and device configurations may be more challenging and multivariate than in photovoltaics. By quantifying technological maturity, we can better target research efforts and accelerate innovation, which will enable transparent technology comparisons, increasing investment and manufacturing readiness. Electrochemical CO2 conversion holds promise for producing fuels and chemicals, yet faces hurdles in scaling to industrial levels. In this Perspective, drawing lessons from photovoltaics, the authors discuss measures to help transition the technology from the laboratory to large-scale deployment.
Gradual reverse-bias breakdown in metal-halide perovskite diodes and solar cells is thought to originate from hole tunneling through steep bands in an ionic depletion region near the electron-transport layer after positively charged iodine vacancies accumulate near the hole-transport layer (HTL). However, typical reported mobile-ion concentrations near 1×1017 cm-3 are too small to quantitatively explain significant tunneling-current densities and (Zener) breakdown observed near −5 V. Here, we show that inferred mobile-ion concentrations increase by more than 100×, to over 1×1018 cm-3, within just 3 min of reverse bias at −6.0 V in p-i-n perovskite diodes. We attribute this increase to iodide oxidation and coupled iodine vacancy creation that must be balanced by reduction reactions near the HTL. Sub-optimal HTL coverage leads to direct contact between the transparent conducting electrode and perovskite, facilitates reduction events, enables the creation of even larger inferred mobile-ion concentrations (∼1×1019 cm-3), and leads to faster degradation under reverse bias. This explains previous work that showed increased breakdown voltages and improved reverse-bias stability by implementing thick, uniform HTLs.
Mixed-halide wide-bandgap (WBG) perovskites needed in tandem photovoltaics suffer from phase segregation, even at the time of initial film formation: the result of asymmetric nucleation of I-rich and Br-rich phases1-3. Known homogenization strategies tune Pb2+ coordination strength4-6; however, Pb2+-based modulation applies across all Pb2+ centres and does not preferentially address the problem that PbBrx nucleates faster than does PbIx. Here we introduce a selective coordination principle: we tune local Lewis-base hardness at the donor atom through a molecular dipole, an approach that constrains the polarizability of the oxygen donor's outermost electrons. The harder oxygen donor preferentially coordinates the harder Pb2+ of PbBrx, selectively retarding Br-rich nucleation and synchronizing it with PbIx. This leads to compositionally homogeneous WBG films, enabling solar cells with bandgaps of 1.62 eV, 1.68 eV and 1.88 eV, each achieving enhanced power conversion efficiency and extended stability (1,500 hours, ≥T90, 1 sun and 65 °C). Perovskite-organic tandem cells fabricated with these WBG films and an infrared-active organic cell deliver certified 27.0% (steady-state 26.4%) efficiency, with T91 (ISOS-L2 at 65 °C) of 1,000 hours.
Since the first demonstration in the early 2010s, perovskite solar cells (PSCs) have emerged as a promising next-generation photovoltaic technology. With power conversion efficiencies improving at a rate of approximately 1% per year, PSCs are approaching energy-efficiency parity with silicon-based photovoltaics. As single-junction efficiency gains begin to plateau, research efforts are increasingly directed towards addressing operating stability while maintaining device performance. Defects and impurities at the interface compromise long-term stability and limit device efficiency. Consequently, interface passivation has emerged as a central focus of the field. We emphasize three emerging strategies to improve how interfaces are constructed and engineered in PSCs: multifunctional passivation molecules suppress non-radiative losses and ion migration through cooperative interactions; heterostructure interfaces modulate band alignment and defect landscapes; and self-assembled monolayers offer molecular control over surface energetics and thin-film growth. These approaches target the root causes of performance loss and together tackle pressing topics in PSCs. Interface engineering is promising for advancing perovskite solar cell (PSC) performance and longevity. This Review highlights three emerging strategies for interfacial optimization in PSCs: multifunctional molecular passivation, heterostructures and self-assembled monolayers. The authors discuss relevant materials, assess their limitations and outline challenges and prospective directions for future research.
Surface defect-induced photoluminescence blinking and photodarkening are ubiquitous in lead halide perovskite quantum dots. Despite efforts to stabilize the surface by chemically engineering ligand binding moieties, blinking accompanied by photodegradation still poses barriers to implementing perovskite quantum dots in quantum emitters. To date, ligand tail engineering in the solid state has rarely been explored for perovskite quantum dots. We posit that attractive intermolecular interactions between low-steric ligand tails, such as π-π stacking, can promote the formation of a nearly epitaxial ligand layer that significantly reduces the quantum dot surface energy. Here, we show that single CsPbBr3 quantum dots covered by stacked phenethylammonium ligands exhibit nearly non-blinking single photon emission with high purity (~ 98%) and extraordinary photostability (12 hours continuous operation and saturated excitations), allowing the determination of size-dependent exciton radiative rates and emission line widths of CsPbBr3 quantum dots at the single particle level. Mi et al. report epitaxial surface coverage of single CsPbBr3 quantum dots with size ranging from 3.6 nm to 14 nm using low steric ligand tails with attractive π-π stacking, leading to nearly non-blinking single photon emission with high purity of 98% and photostability over 12-hour irradiation.
Three-dimensional (3D) perovskites of the formula AMX3 are known for their excellent optoelectronic properties, but their design is limited by the narrow range of A-site cations that can template the 3D corner-sharing structure, and many of the viable options have already been explored. These materials also face structural instability under environmental conditions. In contrast, 3D hexagonal perovskitoids, with the same chemical formula, may offer enhanced stability and richer structural diversity through a range of corner- and face-sharing octahedral configuration options, providing greater opportunities for structural design; however, challenges such as synthesis complexity and wide band gaps have hindered optoelectronic performance achieved to date. Herein, we synthesized a structural homologous series of mixed-metal hexagonal perovskitoids with the formula APb1-xSnxI3 (x = 0, 0.25, 0.50, 0.75, 1; A = ethylammonium, guanidinium) and identified three polytypes (9R, 12R, 6H) using single-crystal X-ray diffraction (SCXRD). These structures exhibited increasing corner-sharing connectivity with higher Sn content, revealing a previously unobserved relationship between metal composition and structural evolution in perovskitoid materials. The incorporation of Sn reduced the band gap (tunable from 2.51 to 1.87 eV) and drove structural transformations, a trend seen also in density functional theory (DFT) calculations, which suggest a thermodynamic preference for Pb at face-sharing sites and Sn at corner-sharing sites. DFT band structure calculations and optical spectroscopy also reveal an anomalous behavior in these materials, which we term polytypic band modulation. This phenomenon combines conventional band bowing with the structural transformations that occur as Sn content increases, as observed in the band gap and in photoluminescence spectra. Photodiodes fabricated from thin films of these materials exhibited stable and pronounced photoresponses across various light intensities over time. The combination of templating 3D perovskitoids with multiple cations and alloying Pb and Sn suggests a vastly underexplored phase space that offers new parameters to tune perovskitoids.
Perovskite solar cells (PSCs) have received more and more attention because they have the following advantages, such as good photoelectric conversion effect, simple preparation process and sufficient raw materials. Laminated PSCs have high power conversion efficiency (PCE), light weight, thin thickness, large flexibility, translucency, good low light effect, color can be customized and so on. But its technological maturity still needs to be improved. The addition of sulfur in chalcogenides may change the structure and performance of perovskites. The introduction of sulfur atoms may affect the crystal structure of perovskites. SCAPS-1D and DFT are used to study the performance of a layered PSCs device with chalcogenide compounds CZTS (Cu2ZnSnS4) and CNGS (Cu2NiGeS4) as absorption layers is provided. The material characteristic of the absorb layer were analyzed and calculated by VASP software, and the property of the cells was optimized by SCAPS-1D. The setting of IDL layer is improved, which provides enlightenment for future work. Innovative applications without etl layers reduce costs while increasing efficiency. The PCE and FF of the optimized structure reached 30.22 % and 82.28 %.In this work, VASPKIT is used to process and analyze the data in the first-principle calculation, and further study the internal mechanism of the absorption layer, which lays a foundation for the further development of the material in the future. What is exciting is that the device has wonderful stability at extreme temperatures. These results indicate that the superposed perovskite solar cells provide inspiration for the work of subsequent researchers.
Fe7S8 with large capacity shows high potential for Li-ion batteries, while it still suffers large volume expansion, resulting in fast capacity fading. Herein, a novel yolk-shell structural Fe7S8@C-N is rationally designed, in which the N-doped carbon layer with superior mechanical flexibility enables one to accommodate the volume expansion of the Fe7S8 core and promote its electronic transportation. Besides, the surface porous morphology is believed to facilitate electrolyte infiltration and Li-ion diffusion as well. Therefore, this modified Fe7S8@C-N electrode exhibits lower expansivity (∼28.0% vs ∼87.4%), smaller voltage hysteresis, higher conductivity (1.6 × 10-2 S/m) and better Li-diffusivity (1.09 × 10-12 cm2/s) than its pure Fe7S8 powder; thus better cyclability (458 mAh/g vs 121 mAh/g after 150 cycles) and rate-capability improvement (546 mAh/g vs 125 mAh/g at 2000 mA/g) can be achieved. Such a yolk-shell structural design strategy can be easily extended to other conversion or alloying type materials for advanced energy storage.
Polymetallic electrocatalysts represent as a promising strategy for steering the electrocatalytic CO2 reduction reactions (eCO2RR) toward valuable products. However, achieving simultaneous high selectivity and activity remains challenging. Here, we report a dual-doped CuO catalyst (CuO-Sn0.02-Ga0.005) that synergistically combines Sn and Ga to achieve exceptional performance for CO2-to-CO conversion. Electrochemical evaluations demonstrate that the optimized catalyst exhibits a Faradaic efficiency (FE) of 99.37 % for CO at -0.7 VRHE with a current density of -132.8 mA cm-2, significantly outperforming pristine CuO (54.21 %, -47.6 mA cm-2 and single-doped counterparts (93.50 %, -55.3 mA cm-2 for CuO-Sn0.02 and 46.76 %, -94.2 mA cm-2 for CuO-Ga0.02, respectively). Sn doping suppresses hydrogen evolution and enhances CO selectivity, while Ga doping boosts catalytic activity. In situ Raman spectroscopy reveals that Sn incorporation facilitates the stabilization of key intermediates (e.g., *COOH), whereas Ga introduces lattice strain and defects, enlarging the electrochemically active surface area. The catalyst also demonstrates remarkable stability, maintaining >95 % FE for CO over 75 h. This work provides a rational design strategy for non-precious metal catalysts through dual-element doping, highlighting the critical role of electronic and structural modulation in eCO2RR.
Inverted p-i-n structure perovskite solar cells (PSCs) have outperformed traditional n-i-p PSCs in recent years. A key advancement is the use of self-assembled monolayers (SAMs) as hole transport layers. One class of widely used SAMs is carbazole-based phosphonic acids. However, it is found that these SAMs lack strong binding with transparent conducting oxides (TCO) and perovskite. The weak binding strength results in suboptimal interfacial adhesion of the buried interface, which limits the device's stability. Here, interfacial binding is enhanced by increasing the dipole moment that creates a strong interfacial electric field that enhances electrostatic interactions at the TCO/perovskite interface, while incorporating tailored functional groups in SAMs to improve chemical anchoring to TCO and binding to perovskite. Specifically, the donor-acceptor SAM molecule 4-(7-(4-(bis(4-methoxyphenyl)amino)-2,5-difluorophenyl)benzo[c][1,2,5]thiadiazol-4-yl)benzoic acid (PAFTB) is employed, which features an enhanced dipole moment along with electron-donating and electron-withdrawing functional groups to optimize interfacial interactions. Compared to extensively used [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz), PAFTB enhances total interfacial adhesion by 2.8 times, thereby improving the thermal stability of the layer. Using this approach, PSCs are demonstrated with a certified quasi-steady-state power conversion efficiency of 24.9% and maintain 80% of the initial efficiency after 900 h of maximum power point tracking at 85 °C.