The unstable Zn interface caused by undesired dendrites and parasitic side reactions greatly impedes the deployment of aqueous Zn metal batteries. Herein, an efficient adsorptive additive strategy is proposed to reshape the electric double layer and regulate Zn interfacial chemistry. 2-Hydroxy-4′-(2-hydroxyethoxy)-2-methylpropiophenone (Irgacure 2959) was selected owing to its strong adsorption ability, intermolecular hydrogen bonding, and exposed strong electronegative carbonyl group. The constructed self-adaptive adlayer contributes to a localized H2O, SO42–-poor environment and horizontal alignment of Zn deposits along the (002) plane, thus endowing thermodynamically stable and highly reversible Zn electrochemistry. As a result, reversible plating/stripping of 3800 h and high Coulombic efficiency of 99.8% are achieved. Intriguingly for practical application, the economical additive (0.016 USD L–1) enables stable discharge output for 500 cycles in Zn/VS2 cells at a low negative-to-positive capacity ratio of 2.5 (cathode mass loading: 10.8 mg cm–2), holding great promise for use in a scalable, low-cost, rechargeable battery.

Lithium metal anodes are crucial for high-energy-density batteries, but concerns regarding their safety remain. Limited investigations have evaluated the reactivity of Li metal anodes in full cell configurations. In this study, differential scanning calorimetry (DSC) and in situ Fourier-transform infrared spectroscopy (FTIR) were employed to quantitatively examine the Li metal reactivity. Lithiated graphite (Li-Gr) and lithiated silicon (Li-Si) were also compared. The reactivity of plated Li was systematically investigated when combined with different electrolyte compositions, morphologies, atmospheres, and various cathode materials (NMC622, LFP, and LNMO). It was discovered that all cell components, such as electrolyte composition, Li morphology, control of inactive Li accumulation, and cathode stability, play essential roles in regulating the reactivity of the plated Li. By optimizing these factors, the Li metal full cell exhibited no significant thermal reaction up to 400 °C. This research identifies key parameters for controlling Li metal reactivity, potentially advancing lithium metal battery design and manufacturing.

Quasi-two-dimensional (2D) Pb–Sn mixed perovskites show great potential in applications of single and tandem photovoltaic devices, but they suffer from low efficiencies due to the existence of horizontal 2D phases. Here, we obtain a record high efficiency of 18.06% based on 2D ⟨n⟩ = 5 Pb–Sn mixed perovskites (iso-BA2MA4(PbxSn1–x)5I16, x = 0.7), by optimizing the crystal orientation through a regulation of the Pb/Sn ratio. We find that Sn-rich precursors give rise to a mixture of horizontal and vertical 2D phases. Interestingly, increasing the Pb content can not only entirely suppress the unwanted horizontal 2D phase in the film but also enhance the growth of vertical 2D phases, thus significantly improving the device performance and stability. It is suggested that an increase of the Pb content in the Pb–Sn mixed systems facilitates the incorporation of iso-butylammonium (iso-BA+) ligands in vertically oriented perovskites because of the reduced lattice strain and increased interaction between the organic ligands and inorganic framework. Our work sheds light on the optimal conditions for fabricating stable and efficient 2D Pb–Sn mixed perovskite solar cells.

Understanding the degradation pathways and reactivity of electrolytes is the key to address the shortcomings of conventional electrolytes and to develop new electrolytes for high-voltage lithium metal batteries (LMBs). Accordingly, while 1,3-dioxolane (DOL) exhibits desired features such as good compatibility with Li metal, low viscosity, and high ionic conductivity, it suffers from poor oxidation stability, mainly from its ring-opening polymerization. In an effort to control the reactivity of DOL by tuning its electronic properties, we introduced methyl and trifluoromethyl groups to the ethyl moiety of DOL and developed 4-methyl-1,3-dioxolane (MDOL) and 4-(trifluoromethyl)-1,3-dioxolane (TFDOL) as solvents, respectively. Whereas the MDOL-based electrolyte exhibited serious side reactions toward metallic Li, the TFDOL-based electrolyte showed oxidation stability up to 5.0 V. Moreover, the inorganic-rich solid electrolyte interphase induced by the weak solvation power of TFDOL along with high oxidation stability enabled a robust cycling stability in a Li|NCM811 full cell (20 μm Li foil, N/P ratio of 2.5).

Sorption-based atmospheric water harvesting (AWH) is regarded as a promising way to produce fresh water in water-stressed areas. However, low water production per unit device mass (WPD) and high energy consumption restrict its applications in portable fresh water replenishment. Here we report a portable high-yield AWH device based on a thermoelectric cell (TEC)-driven integrated heating/cooling thermal design, enabled by a thermally tailored hydrogel sorbent. Heat and cold energies for desorption and condensation are simultaneously generated by the TEC. Graphene oxide-doped sodium alginate hydrogel with high thermal conductivity is tailored as the sorbent, which tightly adheres to the TEC’s hot region and efficiently takes heat away, for fast desorption as well as temperature control of the TEC. Based on the thermal design of the device and materials, a total WPD of 0.18 L kgdevice–1 h–1 is achieved under 80% RH, almost an order of magnitude higher than that of the traditional design with the same energy input.

Gas-fed flow cells can facilitate high-rate electrochemical CO2 reduction (CO2R). However, under alkaline and neutral conditions, CO2 is lost through reaction with hydroxide ions to form (bi)carbonate. In acidic solutions, although (bi)carbonate is still formed due to increased pH at the electrode, the low bulk pH of the electrolyte solution can regenerate CO2 which is then available for re-reaction or release─this therefore avoids permanent CO2 loss. Here, we show how CO2 is converted and released in a bipolar-membrane-based gas-fed flow cell for CO2R to multicarbon products (C2+ faradaic efficiency >60%) employing an acidic catholyte. Under the highest conversion conditions, we showed that almost exclusively CO2R products were obtained at one outlet, while, at the second outlet, a nearly product-free stream of CO2 was obtained due to the continuous internal regeneration from (bi)carbonate. The system presented here avoids permanent reactant loss through the straightforward recovery and recycling of CO2 to improve the overall CO2 utilization.

Using a fast and simple one-step electrochemical method, we developed transparent and conductive ZnO nanoporous layers encapsulating molecular catalysts, showcasing dual functionality as a window layer for thin-film solar cells and a catalytic layer for solar-to-fuel conversion. As a proof of concept, tetraammonium-substituted Co phthalocyanine (CoPcTA) was encapsulated into the window layer of high-efficiency Cu(In,Ga)Se2 (CIGS) solar cells demonstrating photoelectrochemical (PEC) reduction of CO2 into CO with a selectivity of 93% and current densities up to ca. 7 mA cm–2 at −1.7 V vs SCE under 1 sun irradiation, which corresponds to a turnover number (TON) of above 100000 and a turnover frequency (TOF) of 10 s–1 after 3 h. The simplicity and versatility of this approach make the nanoporous catalytic ZnO layer not only easily adaptable to different high-efficiency solar cells but also pave the way for flexible testing of diverse molecular catalysts for CO2 conversion into diverse, valuable fuels.

We report an on-chip light-incorporated in situ transmission electron microscopy (LI2ST) approach for probing metal halide perovskites (MHPs) at the nanoscale, realizing the real-time, site-specific tracking of the light-triggered structure transformation. This in situ platform is based on a specifically designed microelectromechanical systems (MEMS) chip that offers the capability of light illumination with adjustable intensity and tailorable multiwavelength. The excellent operational reliability of the platform allows for the continuous observation of nanoscale regions of interest, recording the morphological and structural evolutions of perovskite grains and grain boundaries. A proof-of-concept demonstration shows a polycrystalline MHP film undergoing decomposition upon continuous light illumination. Counterintuitively, the decomposition starts and expands within the intragrain regions rather than at the grain boundaries. This work demonstrates an unprecedented ability to reveal light-triggered structural-phase variation for illuminating the dynamic behaviors of MHPs with implications for various energy applications.

Potassium shows great potential to replace lithium in energy storage for its high abundance and comparable energy density. However, issues including an unstable interphase, dendrite growth, and volume change restrict the development of potassium metal batteries, and so far, there is no single cure that works once and for all. Here an anode-free potassium metal battery is demonstrated by introducing a customized electrolyte and host structures that simultaneously promote efficiency, reversibility, and energy density. First, a diluted high-concentration electrolyte with fast kinetics and high stability triggers an inorganic-rich durable interphase. Meanwhile, a carbonaceous host containing narrowly distributed mesopores (MCNF) favors reduced surface area but enough inner space. Together, they achieve a high average Coulombic efficiency (CE) of 99.3% and an initial CE of 95.9% at 3 mA cm–2–3 mA h cm–2. Anode-free MCNF||Prussian blue (PB) potassium cells are delivered with 100 reversible cycles and a high energy density of 362 W h kg–1.

Figure 1. The importance of nanomaterials and sustainability to science and technology is schematically illustrated via the interconnections of three topical areas: Nanostructured Materials for Sustainable Energy Solutions, Nano-bio Hybrid Materials for Energy and CO2 Reduction, and Sustainable Manufacturing at the Nanoscale. Figure 2. Diagram showing different pump–probe techniques and the information obtained from each technique. Figure 3. (Top) Assembly of a nano-bio hybrid. (Bottom left) Proposed mechanism of photosynthetic CO2 reduction to value-added chemicals by a nano-bio hybrid. (Bottom right) Photocatalytic CH4 and CO formation under various conditions. Adapted from ref (14). Copyright 2019 American Chemical Society. Figure 4. Schematics of a graphene/nanodiamond-based superlubric solid lubricant coating developed at Argonne National Laboratory showing application from (a) solution to (b) bearing. The schematic in (c) shows a diamond-like carbon (DLC) ball sliding on nanodiamond/graphene patches. Adapted from ref (16). Copyright 2015 American Association for the Advancement of Science. Figure 5. 2030 cumulative iridium demand. Conservative at 80–100 GW at 40% PEM; aggressive at 80% PEM. Work at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Material from P.K.J. is based upon work supported by the National Science Foundation under Grant No. CHE-2304910. The work of H.X. was supported by the U.S. National Science Foundation Grant Nos. DMR-1408949, 1454984, and 1838604. R.B. thanks the Graduate School NANO- PHOT (École Universitaire de Recherche, contract ANR-18-EURE-0013) for support. This article references 20 other publications. This article has not yet been cited by other publications. Figure 1. The importance of nanomaterials and sustainability to science and technology is schematically illustrated via the interconnections of three topical areas: Nanostructured Materials for Sustainable Energy Solutions, Nano-bio Hybrid Materials for Energy and CO2 Reduction, and Sustainable Manufacturing at the Nanoscale. Figure 2. Diagram showing different pump–probe techniques and the information obtained from each technique. Figure 3. (Top) Assembly of a nano-bio hybrid. (Bottom left) Proposed mechanism of photosynthetic CO2 reduction to value-added chemicals by a nano-bio hybrid. (Bottom right) Photocatalytic CH4 and CO formation under various conditions. Adapted from ref (14). Copyright 2019 American Chemical Society. Figure 4. Schematics of a graphene/nanodiamond-based superlubric solid lubricant coating developed at Argonne National Laboratory showing application from (a) solution to (b) bearing. The schematic in (c) shows a diamond-like carbon (DLC) ball sliding on nanodiamond/graphene patches. Adapted from ref (16). Copyright 2015 American Association for the Advancement of Science. Figure 5. 2030 cumulative iridium demand. Conservative at 80–100 GW at 40% PEM; aggressive at 80% PEM. This article references 20 other publications.

Transition metal selenides as electrode materials for supercapacitors are becoming increasingly attractive, and effective modification strategies for improving their practical energy storage performance are highly desired. Herein, a dual modification strategy combined with surface laminating and introducing cation vacancies is utilized to optimize the polynary transition metal selenide CoNiSe2 in the surface and atomic levels. The as-obtained sample CNVS/rGO possesses well-developed surface chemical properties, optimized electron state, more exposed inner electroactive sites, and barrier-decreased kinetics. For the assembled asymmetric hybrid supercapacitor device, a high energy density of 106.2 Wh kg–1 at a power density of 0.77 KW kg–1 is achieved. Importantly, a pseudo-in-situ XPS test method and DFT calculations are conducted for better understanding of the modification mechanisms and electrochemical kinetics. This work presents a performance breakthrough; the corresponding modification strategy and kinetic studies are inspiring for the design of electrode materials in the related fields.

Ultrasound-driven triboelectric nanogenerators (TENGs) were recently proposed as an energy solution technology for a sustainable lifespan of implantable medical devices (IMDs). While the improvement of ultrasound transmission is crucial for achieving high energy generation, research on the material properties of ultrasound-driven TENGs is still in its initial stage. In this work, multifunctional, biocompatible 2-hydroxyethyl methacrylate (HEMA) is suggested as both an encapsulation and triboelectric layer for an implantable, modulus-tunable ultrasound-driven TENG (IMU-TENG). By adjusting the acoustic impedance of HEMA to be suitable for the surrounding environment, the ultrasonic transmission coefficient is about 10 times higher than that of a titanium (Ti) plate. Under in vivo conditions, the IMU-TENG generates sufficient energy to charge a 100 μF capacitor 3.7 times faster than the case with a Ti plate. This strategy of using multifunctional HEMA for high-performance ultrasound-driven TENGs could be a promising energy solution for low-powered IMDs.

Inorganic lead halide perovskites (ILHPs) exhibit a series of phase transitions, and stabilization of the phases with desirable optoelectronic properties remains a major challenge. However, the intrinsic origins of structural instabilities in CsPbX3 (X = Br, I) are still elusive. Herein, the important role of harmonic and anharmonic vibrations in influencing thermodynamic fluctuations of ILHPs was revealed, through combined lattice dynamics and multiphonon theory calculations, and verified by diffraction experiments. Our results demonstrate that the transition between δ- and γ-CsPbI3 is driven by harmonic vibrations, unveiling the mysterious mechanism for stabilizing γ-CsPbI3 via applying strain. Moreover, the successive transitions from the α- to β- and β- to γ-phases of CsPbX3 are driven by anharmonic vibrations. These structural dynamics are strongly coherent with the phonon diffuse scattering, substantially affecting the thermal conductivity and carrier relaxation. This work provides guidelines for maintaining favorable ILHP phases through delicately manipulating their lattice dynamics.

Organic redox-active molecules are promising materials for charge storage in redox-flow batteries (RFBs); however, the development of all-organic RFBs is hindered by material crossover, limited energy density, and poor stability of active materials. Here, ester-substituted bispyridinylidenes are reported as the first examples of intrinsic bipolar molecules that exhibit basically concerted double two-electron redox activity at a potential difference of 1.01 V. All three oxidation states of the pentylester derivative exhibited excellent temporal stability and good solubility in the electrolyte. Testing this active material in symmetric cells, which alleviates crossover issues, revealed good cyclability (fade of 0.025% and 0.35% per cycle for static and flow cells, respectively), capacities of up to 89% of the theoretical value, and Coulombic efficiencies above 99%. Considering previous evidence for active material solubility limits of ∼2 M, and the benefits of a symmetric design, such double concerted multielectron bipolar active materials will be key to developing energy dense organic RFBs.

Batch-to-batch variations remain a challenge for organic photovoltaics (OPVs) that must be solved for widespread commercialization. This work addresses the role of the molecular weight (MW), introducing a new donor polymer PM7-D5 with an extended thiophene bridge compared to that of PM6 or PM7. Devices comprising PM7-D5 and the nonfullerene acceptor L8-BO are relatively insensitive to a significant molecular weight variation and result in OPVs with photoconversion efficiencies (PCEs) of 11.4% and 12.4%, when using polymers with 26 and 125 kDa. We elucidate the origins of the small performance change and systematically address morphology, charge generation, recombination, and extraction, combining optical simulations and experimental techniques. The comprehensive analysis emphasizes the complexity of the photoelectric processes and confirms the high robustness to MW variations of this blend system. Lastly, we review reported blends and suggest systematic research of the structural parameters that lead to an increased robustness to MW changes.

The development of long-term stable Zn anodes capable of operating at high current densities and/or capacities remains a huge challenge. Herein, through the rapid potassium permanganate solution treatment and laser lithography, we have developed a gradient Zn anode (LLP@Treated Zn) with the insulating and hydrophobic passivated-layer at the top and conductive and hydrophilic fresh-zinc-layer at the bottom. This makes the passivation layer prevent the Zn anodes from corrosion and side reactions and induce the preferential deposition of Zn at the bottom of the microchannel without dendrite growth. As a consequence, the LLP@Treated Zn anodes exhibit a stable cycle life for over 700 h at 10 mA cm–2 and 5 mAh cm–2. Moreover, the Zn anodes with different surface morphologies (ring, lattice, etc.) could also be obtained by laser lithography, which proves the flexibility of the pulsed laser lithography strategy in the preparation of battery materials.

Garnet solid-electrolyte-based Li-metal batteries can be used in energy storage devices with high energy densities and thermal stability. However, the tendency of garnets to form lithium hydroxide and carbonate on the surface in an ambient atmosphere poses significant processing challenges. In this work, the decomposition of surface layers under various gas environments is studied by using two surface-sensitive techniques, near-ambient-pressure X-ray photoelectron spectroscopy and grazing incidence X-ray diffraction. It is found that heating to 500 °C under an oxygen atmosphere (of 1 mbar and above) leads to a clean garnet surface, whereas low oxygen partial pressures (i.e., in argon or vacuum) lead to additional graphitic carbon deposits. The clean surface of garnets reacts directly with moisture and carbon dioxide below 400 and 500 °C, respectively. This suggests that additional CO2 concentration controls are needed for the handling of garnets. By heating under O2 along with avoiding H2O and CO2, symmetric cells with less than 10 Ωcm2 interface resistance are prepared without the use of any interlayers; plating currents of >1 mA cm–2 without dendrite initiation are demonstrated.

With the advent of nonfullerene acceptors (NFAs), organic photovoltaic (OPV) devices are now achieving high enough power conversion efficiencies (PCEs) for commercialization. However, these high performances rely on active layers processed from petroleum-based and toxic solvents, which are undesirable for mass manufacturing. Here, we demonstrate the use of biorenewable 2-methyltetrahydrofuran (2MeTHF) and cyclopentyl methyl ether (CPME) solvents to process donor: NFA-based OPVs with no additional additives in the active layer. Furthermore, to reduce the overall carbon footprint of the manufacturing cycle of the OPVs, we use polymeric donors that require a few synthetic steps for their synthesis, namely, PTQ10 and FO6-T, which are blended with the Y-series NFA Y12. High performance was achieved using 2MeTHF as the processing solvent, reaching PCEs of 14.5% and 11.4% for PTQ10:Y12 and FO6-T:Y12 blends, respectively. This work demonstrates the potential of using biorenewable solvents without additives for the processing of OPV active layers, opening the door to large-scale and green manufacturing of organic solar cells.

Introduction of interstitial dopants has opened a new pathway to optimize nanoparticle catalytic activity for, e.g., hydrogen evolution/oxidation and other reactions. Here, we discuss the stability of a property-enhancing dopant, B, introduced through the controlled synthesis of an electrocatalyst Pd aerogel. We observe significant removal of B after the hydrogen oxidation reaction. Ab initio calculations show that the high stability of subsurface B in Pd is substantially reduced when H is adsorbed/absorbed on the surface, favoring its departure from the host nanostructure. The destabilization of subsurface B is more pronounced, as more H occupies surface sites and empty interstitial sites. We hence demonstrate that the H2 fuel itself favors the microstructural degradation of the electrocatalyst and an associated drop in activity.

Two-dimensional (2D) tin (Sn2+)-based perovskites have achieved remarkable advancements in (opto)electronic devices. However, fabricating high-quality and reproducible Sn halide perovskite thin films remains challenging due to uncontrollably fast crystallization. To overcome this issue, dimethyl sulfoxide has been incorporated as an indispensable strategy to form Lewis acid–base adducts but also has been proven to induce an irreversible Sn2+ oxidization effect. As the crystalline films grow directly from solution, a better understanding of precursor colloidal chemistry and the film formation process is critical. In this study, we report a universal solution aging approach to fabricate high-quality and reliable 2D Ruddlesden–Popper and Dion–Jacobson Sn2+ perovskite films and devices. The proper solution aging stabilizes the precursor colloids by eliminating aggregated complex and unreacted precursor clusters in the fresh precursor, leading to homogeneous nucleation/crystallization and film growth. The precursor aging reduced film defect density by nearly 2 orders of magnitude and improved charge transport mobility by over 5 times. This study can inspire the community to understand the deposition mechanism for high-quality Sn2+ perovskite thin films and promote the development of high-performance and reproducible Sn2+ perovskite based (opto)electronic devices.