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The photoconversion of CO2 into valuable chemical products using solar energy is a promising strategy to address both energy and environmental challenges. However, the strongly adsorbed CO2 frequently impedes the seamless advancement of the subsequent reaction by significantly increasing the reaction activation energy. Here, we present a BiFeO3 material with lattice strain that collaboratively regulates the d/p-2π* orbitals hybridization between metal sites and *CO2 as well as *COOH intermediates to achieve rapid conversion of solidly adsorbed CO2 to critical *COOH intermediates, accelerating the overall CO2 reduction kinetics. Quasi in-situ X-ray photoelectron spectroscopy and in-situ Fourier Transform infrared spectroscopy combined with theoretical calculation reveals that the optimized Fe sites enhance the adsorption and activation effect of CO2, and continuous internal electrons are rapidly transferred to the reaction sites and injected into the surface *CO2 and *COOH under the condition of illumination, which promotes the rapid formation and stability of *COOH. Certainly, the performance of CO2 photoreduction to CO is improved by 12.81-fold compared with the base material. This work offers a new perspective for the rapid photoreduction process of strongly adsorbed CO2., (© 2024 Wiley‐VCH GmbH.)

Developing anode-free batteries is the ultimate goal in pursuit of high energy density and safety. It is more urgent for sodium (Na)-based batteries due to its inherently low energy density and safety hazards induced by highly reactive Na metal anodes. However, there is no electrolyte that can meet the demanding Na plating-stripping Coulomb efficiency (CE) while resisting oxidative decomposition at high voltages for building stable anode-free Na batteries. Here, a "liquid-in-solid" electrolyte design strategy is proposed to integrate target performances of liquid and solid-state electrolytes. Breaking through the Na + transport channel of Na-containing zeolite molecular sieve by ion-exchange and confining aggregated liquid ether electrolytes in the nanopore and void of zeolites, it achieves excellent high-voltage stability enabled by solid-state zeolite electrolytes, while inheriting the ultra-high CE (99.84%) from liquid ether electrolytes. When applied in a 4.25 V-class anode-free Na battery, an ultra-high energy density of 412 W h kg -1 (based on the active material of both cathodes and anodes) can be reached, which is comparable to the state-of-the-art graphite||LiNi 0.8 Co 0.1 Mn 0.1 O 2 lithium-ion batteries. Furthermore, the assembled anode-free pouch cell exhibits excellent cycling stability, and a high capacity retention of 89.2% can be preserved after 370 cycles., (© 2024 Wiley‐VCH GmbH.)

Photocatalytic oxygen reductive H 2 O 2 production is a promising approach to alternative industrial anthraquinone processes while suffering from the requirement of pure O 2 feedstock for practical application. Herein, we report a spaced double hydrogen bond (IC-H-bond) through multi-component Radziszewski reaction in an imidazole poly-ionic-liquid composite (SI-PIL-TiO 2 ) and levofloxacin hydrochloride (LEV) electron donor for highly efficient and selective photocatalytic air reductive H 2 O 2 production. It is found that the IC-H-bond formed by spaced imino (-NH-) group of SI-PIL-TiO 2 and carbonyl (-C=O) group of LEV can switch the imidazole active sites characteristic from a covered state to a fully exposed one to shield the strong adsorption of electron donor and N 2 in the air, and propel an intenser positive potential and more efficient orbitals binding patterns of SI-PIL-TiO 2 surface to establish competitive active sites for selectivity O 2 chemisorption. Moreover, the high electron enrichment of imidazole as an active site for the 2e - oxygen reduction ensures the rapid reduction of O 2 . Therefore, the IC-H-bond enables a total O 2 utilization and conversion efficiency of 94.8 % from direct photocatalytic air reduction, achieving a H 2 O 2 production rate of 1518 μmol/g/h that is 16 and 23 times compared to poly-ionic-liquid composite without spaced imino groups (PIL-TiO 2 ) and TiO 2 , respectively., (© 2024 Wiley‐VCH GmbH.)

Facile synthesis of hierarchically porous metal-organic frameworks (MOFs) with adjustable porosity and high crystallinity attracts great attention yet remains challenging. Herein, a micromolar amount of dye-based modulator (Rhodamine B (RhB)) is employed to easily and controllably tailor the pore size of a Ti-based metal-organic framework (MIL-125-NH 2 ). The RhB used in this method is easily removed by washing or photodegradation, avoiding secondary posttreatment. It is demonstrated that the carboxyl functional group and the steric effects of RhB are indispensable for enlarging the pore size of the MIL-125-NH 2 . The resulting hierarchically porous MIL-125-NH 2 (RH-MIL-125-NH 2 ) exhibits optimized adsorption and photocatalytic activity because the newly formed mesopore with defects concurrently facilitates mass transport of guest molecules (toluene) and photogenerated charge separation. This work offers a meaningful basis for the construction of hierarchically porous MOFs and demonstrates the superiority of the hierarchical pore structure for adsorption and heterogeneous catalysis., (© 2023 Wiley-VCH GmbH.)

Changing the solvation sheath of hydrated Zn ions is an effective strategy to stabilize Zn anodes to obtain a practical aqueous Zn-ion battery. However, key points related to the rational design remain unclear including how the properties of the solvent molecules intrinsically regulate the solvated structure of the Zn ions. This study proposes the use of a stability constant (K), namely, the equilibrium constant of the complexation reaction, as a universal standard to make an accurate selection of ligands in the electrolyte to improve the anode stability. It is found that K greatly impacts the corrosion current density and nucleation overpotential. Following this, ethylene diamine tetraacetic acid with a superhigh K effectively suppresses Zn corrosion and induces uniform Zn-ion deposition. As a result, the anode has an excellent stability of over 3000 h. This work presents a general principle to stabilize anodes by regulating the solvation chemistry, guiding the development of novel electrolytes for sustainable aqueous batteries., (© 2022 Wiley-VCH GmbH.)

The sodium (Na)-metal batteries hold great promise as a sustainable technology owing to the high element abundance and low cost. However, the generally used carbonate electrolytes remain highly reactive towards Na metal, leading to flammable gas evolution. Here, we propose an electrolyte sieving strategy to separate anion-mediated ion-pairs from dilute electrolytes by introducing a 3A zeolite molecular sieve film. The anion-mediated ion-pair firstly weakens the electron-withdrawing property of the cation, which effectively suppresses the gassing. In addition, the sieved electrolyte promotes the formation of robust inorganic-dominated solid electrolyte interphases. Therefore, it contributes to stable Na plating/stripping in Na|Al half cells with Coulombic efficiency maintaining at 98.5 % and a long service life of 800 cycles in full cells. Moreover, the electrode stability is well preserved even under harsh conditions of high temperature and ester-based electrolytes with higher reactivity., (© 2022 Wiley-VCH GmbH.)

Low-cost and scalable sodium ion (Na-ion) batteries serve as an ideal alternative to the current lithium-ion batteries. To compensate for the shortage of energy density, the most accessible solution is developing a high-voltage anode-free configuration comprising a lightweight Al current collector on the anode and a high-voltage sodiumized cathode. However, it imposes stringent Na reversibility and high-voltage stability requirements on the electrolyte. A 3A zeolite molecular sieve film is rationally designed, and a highly aggregated solvation structure is constructed through the size effect. It suppresses the trace but continuous oxidative decomposition and extends the oxidative stability to 4.5 V without sacrificing the Na reversibility of the anode (99.91 %). Thus, we can make anode-free cells with high energy density of 369 and 372 W h kg -1 for 4.0 and 4.25 V class cells, respectively. Furthermore, this strategy enables a long lifespan (250 cycles) for 4.0 V-class anode-free cells., (© 2022 Wiley-VCH GmbH.)

Alkali metals have low potentials and high capacities, making them ideal anodes for next-generation batteries, but they suffer major problems, including dendrite growth and low Coulombic efficiency (CE). Achieving uniform metal deposition and having a reliable solid electrolyte interphase (SEI) are the basic requirements for overcoming these problems. Here, a general remedy is reported for various alkali-metal anodes by the supramolecularization of alkali-metal cations with crown ethers that follows a size-matching rule. The positively charged supramolecular complex provides electrostatic shielding layers to regulate metal deposition and suppress dendrite formation. More promisingly, it reforms electric double layers and drives the production of organic-dominated SEIs with improved flexibility that can accommodate large volume changes. The high flexibility of SEIs during metal deposition and dissolution reduces the amount of dead metal and improves CE and cycling stability. Specifically, a 200% excess Li-based full cell has a capacity retention of ≈100% after 100 cycles. This crown-like supramolecularization strategy is a new chemistry that may be used for the production of dendrite-free metal-anode-based batteries not limited to the cases with alkali metal. It is also expected as a practical technology to improve the uniformity of coatings produced in the electrodeposition industry., (© 2021 Wiley-VCH GmbH.)

A competitive complexation strategy has been developed to construct a novel electrocatalyst with Zn-Co atomic pairs coordinated on N doped carbon support (Zn/CoN-C). Such architecture offers enhanced binding ability of O 2 , significantly elongates the O-O length (from 1.23 Å to 1.42 Å), and thus facilitates the cleavage of O-O bond, showing a theoretical overpotential of 0.335 V during ORR process. As a result, the Zn/CoN-C catalyst exhibits outstanding ORR performance in both alkaline and acid conditions with a half-wave potential of 0.861 and 0.796 V respectively. The in situ XANES analysis suggests Co as the active center during the ORR. The assembled zinc-air battery with Zn/CoN-C as cathode catalyst presents a maximum power density of 230 mW cm -2 along with excellent operation durability. The excellent catalytic activity in acid is also verified by H 2 /O 2 fuel cell tests (peak power density of 705 mW cm -2 )., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Durability is still one of the key obstacles for the further development of photocatalytic energy-conversion systems, especially low-dimensional ones. Encouragingly, recent studies show that nanoinsulators such as SiO 2 and MgO exhibit substantially enhanced photocatalytic durability than the typical semiconductor p25 TiO 2 . Extending this knowledge, MgO-Au plasmonic defect nanosystems are developed that combine the stable photoactivity from MgO surface defects with energy-focusing plasmonics from Au nanoparticles (NPs), where Au NPs are anchored onto monodispersed MgO nanotemplates. Theoretical calculations reveal that the midgap defect (MGD) states in MgO are generated by oxygen vacancies, which provide the main avenues for upward electron transitions under photoexcitation. These electrons drive stable proton photoreduction to H 2 gas via water splitting. A synergistic interaction between Au's localized plasmons and MgO's oxygen vacancies is observed here, which enhances MgO's photoactivity and stability simultaneously. Such co-enhancement is attributed to the stable longitudinal-plasmon-free Au NPs, which provide robust hot electrons capable of overcoming the interband transition barrier (≈1.8 eV) to reach proton reduction potential for H 2 generation. The demonstrated plasmonic defect nanosystems are expected to open a new avenue for developing highly endurable photoredox systems for the integration of multifunctionalities in energy conversion, environmental decontamination, and climate change mitigation., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A unique CdS/C@Fe3O4 nanoreactor was fabricated by the surface-imprinting technique, which effectively enhances the recyclability, stability, and selectivity for orientation recognition and photodegradation of ciprofloxacin in the binary mixed solution under visible-light irradiation. This work not only puts forward a novel design idea that develops the potential application value of CdS, but also provides a new approach for inhibiting its secondary pollution., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Ink-jet printing of thermoelectric nanomaterials is successfully used to fabricate flexible thin film TE devices for power generation and cooling.

Materials with ordered mesoporous structures have shown great potential in a wide range of applications. In particular, the combination of mesoporosity, low dimensionality, and well-defined morphology in nanostructures may exhibit even more attractive features. However, the synthesis of such structures is still challenging in polar solvents. Herein, we report the preparation of ultrathin two-dimensional (2D) nanoflakes of transition-metal phosphates, including FePO4, Mn3(PO4)2, and Co3(PO4)2, with highly ordered mesoporous structures in a nonpolar solvent. The as-obtained nanoflakes with thicknesses of about 3.7 nm are constructed from a single layer of parallel-packed pore channels. These uniquely ordered mesoporous 2D nanostructures may originate from the 2D assembly of cylindrical micelles formed by the amphiphilic precursors in the nonpolar solvent. The 2D mesoporous FePO4 nanoflakes were used as the cathode for a lithium-ion battery, which exhibits excellent stability and high rate capabilities., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Three dimensional (3D) ordered hierarchically porous electrodes with an entrapped active nanoparticles configuration afford an extremely effective conductive 3D network from the micrometer to the nano meter scale for fast electron and Li-ion transport, and also allow the development of a stable solid electrolyte interphase over the electrode materials, therefore exhibiting extraordinary rate capabilities., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Ultrathin single-crystalline V2 O5 ·0.76H2 O nanosheets with a thickness of 1.5-2.6 nm are prepared on the basis of molecular-level 'oriented attachment' through special sol-gel chemistry. The initial formation of 3-7 nm nanodiscs by confining the condensation reactions within the ab plane is critical to form nanosheets. As a proof-of-concept, these nanosheets exhibit good properties for hydrogen sensors and supercapacitors., (Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)