For the first time, a multi-anionic and multi-cationic high entropy oxyhalide is presented as high capacity cathode for Li-ion batteries.

application-oriented research like process engineering and upscaling is observed. [1][2][3][4][5] Even though other optoelectronic devices like light emitting diodes and lasers are being researched, [6][7][8][9][10][11][12][13] perovskite-based photovoltaics (PV) is the key technology driving the fast emergence of perovskitebased optoelectronics. Recently, power conversion efficiencies (PCEs) close to 24% were demonstrated for perovskite PV, exceeding the PCEs of established thinfilm technologies. [14] Despite the rapid progress in terms of PCE, one key challenge of perovskite-based PV is still its low stability under realistic outdoor stress conditions-temperature, humidity, and ultraviolet (UV) radiation. A significant advance toward more stable devices was demonstrated by engineering the composition of the large cation site of the perovskite crystal structure and by including low-dimensional perovskite interlayers and passivation layers. [15][16][17][18][19][20] Further advances in stability are based on the charge extracting materials and their interfaces with the perovskite absorber layers. [21][22][23] Most reported record PCEs are still based on highly expensive organic hole transport layer (HTL) materials like 2,2′,7,7′-tetrakis[N,N-di (4methoxyphenyl)amino]-9,9′-spirobifluorene (spiro-MeOTAD) or poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA). [20,24,25] Although these materials result in good performance on short High-quality charge carrier transport materials are of key importance for stable and efficient perovskite-based photovoltaics. This work reports on electron-beam-evaporated nickel oxide (NiO x ) layers, resulting in stable power conversion efficiencies (PCEs) of up to 18.5% when integrated into solar cells employing inkjet-printed perovskite absorbers. By adding oxygen as a process gas and optimizing the layer thickness, transparent and efficient NiOx hole transport layers (HTLs) are fabricated, exhibiting an average absorptance of only 1%. The versatility of the material is demonstrated for different absorber compositions and deposition techniques. As another highlight of this work, all-evaporated perovskite solar cells employing an inorganic NiO x HTL are presented, achieving stable PCEs of up to 15.4%. Along with good PCEs, devices with electron-beam-evaporated NiO x show improved stability under realistic operating conditions with negligible degradation after 40 h of maximum power point tracking at 75 °C. Additionally, a strong improvement in device stability under ultraviolet radiation is found if compared to conventional perovskite solar cell architectures employing other metal oxide charge transport layers (e.g., titanium dioxide). Finally, an all-evaporated perovskite solar mini-module with a NiO x HTL is presented, reaching a PCE of 12.4% on an active device area of 2.3 cm 2 .

Monolithic all-perovskite tandem photovoltaics promise to combine low-cost and high-efficiency solar energy harvesting with the advantages of all-thin-film technologies. To date, laboratory-scale all-perovskite tandem solar cells have only been fabricated using non-scalable fabrication techniques. In response, this work reports on laser-scribed all-perovskite tandem modules processed exclusively with scalable fabrication methods (blade coating and vacuum deposition), demonstrating power conversion efficiencies up to 19.1% (aperture area, 12.25 cm2; geometric fill factor, 94.7%) and stable power output. Compared to the performance of our spin-coated reference tandem solar cells (efficiency, 23.5%; area, 0.1 cm2), our prototypes demonstrate substantial advances in the technological readiness of all-perovskite tandem photovoltaics. By means of electroluminescence imaging and laser-beam-induced current mapping, we demonstrate the homogeneous current collection in both subcells over the entire module area, which explains low losses (<5%rel) in open-circuit voltage and fill factor for our scalable modules.

As promising cathode materials, the lithium‐excess 3d‐transition‐metal layered oxides can deliver much higher capacities (>250 mAh g−1 at 0.1 C) than the current commercial layered oxide materials (≈180 mAh g−1 at 0.1 C) used in lithium ion batteries. Unfortunately, the original formation mechanism of these layered oxides during synthesis is not completely elucidated, that is, how is lithium and oxygen inserted into the matrix structure of the precursor during lithiation reaction? Here, a promising and practical method, a coprecipitation route followed by a microwave heating process, for controllable synthesis of cobalt‐free lithium‐excess layered compounds is reported. A series of the consistent results unambiguously confirms that oxygen atoms are successively incorporated into the precursor obtained by a coprecipitation process to maintain electroneutrality and to provide the coordination sites for inserted Li ions and transition metal cations via a high‐temperature lithiation. It is found that the electrochemical performances of the cathode materials are strongly related to the phase composition and preparation procedure. The monoclinic layered Li[Li0.2Ni0.2Mn0.6]O2 cathode materials with state‐of‐the‐art electrochemical performance and comparably high discharge capacities of 171 mAh g−1 at 10 C are obtained by microwave annealing at 750 °C for 2 h.

Layered Delafossite-type Lix(M1M2M3M4M5…Mn)O2 materials, a new class of high-entropy oxides, were synthesized by nebulized spray pyrolysis and subsequent high-temperature annealing. Various metal species (M = Ni, Co, Mn, Al, Fe, Zn, Cr, Ti, Zr, Cu) could be incorporated into this structure type, and in most cases, single-phase oxides were obtained. Delafossite structures are well known and the related materials are used in different fields of application, especially in electrochemical energy storage (e.g., LiNixCoyMnzO2 [NCM]). The transfer of the high-entropy concept to this type of materials and the successful structural replication enabled the preparation of novel compounds with unprecedented properties. Here, we report on the characterization of a series of Delafossite-type high-entropy oxides by means of TEM, SEM, XPS, ICP-OES, Mössbauer spectroscopy, XRD including Rietveld refinement analysis, SAED and STEM mapping and discuss about the role of entropy stabilization. Our experimental data indicate the formation of uniform solid-solution structures with some Li/M mixing.

Interfacial engineering is the key to high‐performance perovskite solar cells (PSCs). While a wide range of fullerene interlayers are investigated for Pb‐based counterparts with a bandgap of >1.5 eV, the role of fullerene interlayers is barely investigated in Sn‐Pb mixed narrow‐bandgap (NBG) PSCs. In this work, two novel solution‐processed fullerene derivatives are investigated, namely indene‐C60‐propionic acid butyl ester and indene‐C60‐propionic acid hexyl ester (IPH), as the interlayers in NBG PSCs. It is found that the devices with IPH‐interlayer show the highest performance with a remarkable short‐circuit current density of 30.7 mA cm−2 and a low deficit in open‐circuit voltage. The reduction in voltage deficit down to 0.43 V is attributed to reduced non‐radiative recombination that the authors attribute to two aspects: 1) a higher conduction band offset of ≈0.2 eV (>0 eV) that hampers charge‐carrier‐back‐transfer recombination; 2) a decrease in trap density at the perovskite/interlayer/C60 interfaces that results in reduced trap‐assisted recombination. In addition, incorporating the IPH interlayer enhances charge extraction within the devices that results in considerable enhancement in short‐circuit current density. Using a NBG device with an IPH interlayer, a respectable power conversion efficiency of 24.8% is demonstrated in a four‐terminal all‐perovskite tandem solar cell.

The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/aenm.202103090.

Active Li-ion battery materials are typically characterized using X-ray photoelectron spectroscopy when regarding chemical state elucidation. This work presents a multiplet-splitting approach comprising in minimum 3 third-row transition metals, namely, Mn, Co, and Ni, to improve the results in comparison to peak barycenter or single symmetric Voigt profile approaches. The achieved X-ray photoelectron spectroscopy 2p templates in particular address the complex peak structures consisting of significant photoelectron multiplet splitting, shake-up and plasmon loss features, and additional Auger and photoelectron overlaps, inevitable also for a reliable quantification. To separate from topography effects and contributions of the electrode's binder and conductive carbon in powder electrodes, the developed procedure in a first attempt was successfully transferred to novel radio frequency magnetron sputtered Li-Ni-Co-Mn-O thin films, designed for all-solid-state Li-ion batteries. In all cases, special care was taken with respect to air sensitivity, contamination during sample handling, and probable method induced sample decomposition. Composition and origin of the anode's surface electrolyte interphase are rather complicated, and therefore, XPS and time-of-flight secondary ion mass spectrometry results are still controversially discussed. [5][6][7][8][9][10][11] However, in the case of the first-row transition metals, which are commonly used in LIB's cathodes, the analytical potential of XPS is not widely used in its entirety. Obviously, the major reason for this fact is mainly due to the complex multiplet splitting, peak overlaps, and additional shake-up and plasmon features in the respective 2p XP spectra, although fundamental studies are available mainly by the work of Biesinger et al, 12 who considered a semiempirical approach combining the analysis of high purity oxide/hydroxide reference samples and theoretically calculated free-ion multiplet structures of core 2p vacancy levels by Gupta and Sen. 13 Aside presenting only raw data sets and solely assigning expected oxidation states, [14][15][16][17][18][19][20] simplifying approaches such as reducing the complex multiplet splitting to single Voigt peak shapes are often used, which, in consequence, could lead at least to uncertainties in the quantitative chemical information. 17,[21][22][23][24] To the best of our knowledge, only a few groups apply complex multiplet fitting procedures during XPS characterization of LIB active materials. 25,26