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Abstract Sodium‐storage performance of pyrite FeS2 is greatly improved by constructing various FeS2‐based nanostructures to optimize its ion‐transport kinetics and structural stability. However, less attention has been paid to rapid capacity degradation and electrode failure caused by the irreversible phase‐transition of intermediate NaxFeS2 to FeS2 and polysulfides dissolution upon cycling. Under the guidance of theoretical calculations, coupling FeS2 nanoparticles with honeycomb‐like nitrogen‐doped carbon (NC) nanosheet supported single‐atom manganese (SAs Mn) catalyst (FeS2/SAs Mn@NC) via atomic‐interface engineering is proposed to address above challenge. Systematic electrochemical analyses and theoretical results unveil that the functional integration of such two type components can significantly enhance ionic conductivity, accelerate charge transfer efficiency, and improve Na+‐adsorption capability. Particularly, SAs Mn@NC with Mn‐Nx coordination center can reduce the decomposition barrier of Na2S and NaxFeS2 to further accelerate reversible phase transformation of Fe/Na2S→NaFeS2→FeS2 and polysulfides decomposition. As predicted, such FeS2/SAs Mn@NC showcases outstanding rate capability and fascinating cyclic durability. A sequence of kinetic studies and ex situ characterizations provide the comprehensive understanding for ion‐transport kinetics and phase‐transformation process. Its practical use is further demonstrated in sodium‐ion full cell and capacitor with impressive electrochemical capability and excellent energy‐density output.

Abstract Electrocatalytic H2 production from seawater, recognized as a promising technology utilizing offshore renewables, faces challenges from chloride-induced reactions and corrosion. Here, We introduce a catalytic surface where OH– dominates over Cl– in adsorption and activation, which is crucial for O2 production. Our NiFe-based anode, enhanced by nearby Cr sites, achieves low overpotentials and selective alkaline seawater oxidation. It outperforms the RuO2 counterpart in terms of lifespan in scaled-up stacks, maintaining stability for over 2500 h in three-electrode tests. Ex situ/in situ analyses reveal that Cr(III) sites enrich OH–, while Cl– is repelled by Cr(VI) sites, both of which are well-dispersed and close to NiFe, enhancing charge transfer and overall electrode performance. Such multiple effects fundamentally boost the activity, selectively, and chemical stability of the NiFe-based electrode. This development marks a significant advance in creating durable, noble-metal-free electrodes for alkaline seawater electrolysis, highlighting the importance of well-distributed catalytic sites.

Abstract It is vital to explore effective ways for prolonging electrode lifespans under harsh electrolysis conditions, such as high current densities, acid environment, and impure water source. Here we report alternating electrolysis approaches that realize promptly and regularly repair/maintenance and concurrent bubble evolution. Electrode lifespans are improved by co-action of Fe group elemental ions and alkali metal cations, especially a unique Co2+-Na+ combo. A commercial Ni foam sustains ampere-level current densities alternatingly during continuous electrolysis for 93.8 h in an acidic solution, whereas such a Ni foam is completely dissolved in ~2 h for conventional electrolysis conditions. The work not only explores an alternating electrolysis-based system, alkali metal cation-based catalytic systems, and alkali metal cation-based electrodeposition techniques, and beyond, but demonstrates the possibility of prolonged electrolysis by repeated deposition-dissolution processes. With enough adjustable experimental variables, the upper improvement limit in the electrode lifespan would be high.

Abstract Seawater electroreduction is attractive for future H2 production and intermittent energy storage, which has been hindered by aggressive Mg2+/Ca2+ precipitation at cathodes and consequent poor stability. Here we present a vital microscopic bubble/precipitate traffic system (MBPTS) by constructing honeycomb-type 3D cathodes for robust anti-precipitation seawater reduction (SR), which massively/uniformly release small-sized H2 bubbles to almost every corner of the cathode to repel Mg2+/Ca2+ precipitates without a break. Noticeably, the optimal cathode with built-in MBPTS not only enables state-of-the-art alkaline SR performance (1000-h stable operation at –1 A cm−2) but also is highly specialized in catalytically splitting natural seawater into H2 with the greatest anti-precipitation ability. Low precipitation amounts after prolonged tests under large current densities reflect genuine efficacy by our MBPTS. Additionally, a flow-type electrolyzer based on our optimal cathode stably functions at industrially-relevant 500 mA cm−2 for 150 h in natural seawater while unwaveringly sustaining near-100% H2 Faradic efficiency. Note that the estimated price (~1.8 US$/kgH2) is even cheaper than the US Department of Energy’s goal price (2 US$/kgH2).

Abstract The development of highly efficient sodium‐ion batteries depends critically on the successful exploitation of advanced anode hosts that is capable of overcoming sluggish reaction kinetics while also withstanding severe structural deformation triggered by the large radius of Na+‐insertion. Herein, a hierarchically hybrid material with hetero‐Co3S4/NiS hollow nanosphere packaged into a densified N‐doped carbon matrix (Co3S4/NiS@N‐C) was designed and fabricated utilizing CoNi‐glycerate as the self‐sacrifice template, making the utmost of the synergistic effect of hetero‐Co3S4/NiS with strong electric field and rich reaction active‐sites together with the densified outer‐carbon scaffolds with remarkable electronic conductivity and robust mechanical toughness. As anticipated, as‐fabricated Co3S4/NiS@N‐C anode affords remarkable specific capacity, prolonged cycle lifespan up to 2 400 cycles with an only 0.05% fading each cycle at 20.0 A g−1, and excellent rate feature (354.9 mAh g−1 at 30.0 A g−1), one of the best performances for most existing Co3S4/NiS‐based anodes. Ex situ structural characterizations in tandem with theoretical analysis demonstrate the reversible insertion‐conversion mechanism of initially proceeding with Na+ de‐/intercalation and superior heterogeneous interfacial reaction behavior with strong Na+‐adsorption ability. Further, sodium‐ion full cell and hybrid capacitor based on Co3S4/NiS@N‐C anode exhibit impressive electrochemical characteristics on cycling performance and rate capability, showcasing its outstanding feasibility toward practical use.

Abstract The electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality and reduce environmental pollution, but also establishes a route to synthesize valuable chemicals, such as urea, amide, and amine. This innovative approach expands the application range and product categories beyond simple carbonaceous species in electrocatalytic CO2 reduction, which is becoming a rapidly advancing field. This review summarizes the research progress in electrocatalytic urea synthesis, using N2, NO2−, and NO3− as nitrogenous species, and explores emerging trends in the electrosynthesis of amide and amine from CO2 and nitrogen species. Additionally, the future opportunities in this field are highlighted, including electrosynthesis of amino acids and other compounds containing C–N bonds, anodic C–N coupling reactions beyond water oxidation, and the catalytic mechanism of corresponding reactions. This critical review also captures the insights aimed at accelerating the development of electrochemical C–N coupling reactions, confirming the superiority of this electrochemical method over the traditional techniques.

Summary: Herein, a hierarchical NiTe@NiFe-LDH core-shell array on Ni foam (NiTe@NiFe-LDH/NF) demonstrates its effectiveness for oxygen evolution reaction (OER) in alkaline seawater electrolyte. This NiTe@NiFe-LDH/NF array showcases remarkably low overpotentials of 277 mV and 359 mV for achieving current densities of 100 and 500 mA cm−2, respectively. Also, it shows a low Tafel slope of 68.66 mV dec−1. Notably, the electrocatalyst maintains robust stability over continuous electrolysis for at least 50 h at 100 mA cm−2. The remarkable performance and hierarchical structure advantages of NiTe@NiFe-LDH/NF offer innovative insights for designing efficient seawater oxidation electrocatalysts.

Summary: Electrochemical reduction of nitrite (NO2−) can satisfy the necessity for NO2− contaminant removal and deliver a sustainable pathway for ammonia (NH3) generation. Its practical application yet requires highly efficient electrocatalysts to boost NH3 yield and Faradaic efficiency (FE). In this study, CoP nanoparticle-decorated TiO2 nanoribbon array on Ti plate (CoP@TiO2/TP) is verified as a high-efficiency electrocatalyst for the selective reduction of NO2− to NH3. When measured in 0.1 M NaOH with NO2−, the freestanding CoP@TiO2/TP electrode delivers a large NH3 yield of 849.57 μmol h−1 cm−2 and a high FE of 97.01% with good stability. Remarkably, the subsequently fabricated Zn–NO2− battery achieves a high power density of 1.24 mW cm−2 while delivering a NH3 yield of 714.40 μg h−1 cm−2.

Abstract Electrochemical nitrate (NO3−) reduction is a green and economic route for ammonia (NH3) synthesis. However, this conversion suffers from low NH3 selectivity due to strong competition from other NO3− reduction pathways. Here, we report that a plasma‐induced defective CoTiO3 − x nanofiber with oxygen vacancies acts as an efficient electrocatalyst for NO3− reduction to NH3. In 0.1 M NaOH solution containing 0.1 M NO3−, it is capable of achieving a remarkable NH3 yield of 30.4 mg h–1 mgcat.–1 and a high Faradaic efficiency of 92.6%. The catalyst also shows strong electrochemical stability for a 20‐h electrolysis test. Additionally, a Zn‐NO3− battery using CoTiO3 − x as the cathode catalyst offers a peak power density of 5.04 mW cm−2 and a large NH3 yield of 3.08 mg h−1 mgcat.−1. The catalytic mechanism is further discussed by density functional theory calculations.

Seawater electrolysis is an extremely attractive approach for harvesting clean hydrogen energy, but detrimental chlorine species (i.e., chloride and hypochlorite) cause severe corrosion at the anode. Here, we report our recent finding that benzoate anions-intercalated NiFe-layered double hydroxide nanosheet on carbon cloth (BZ-NiFe-LDH/CC) behaves as a highly efficient and durable monolithic catalyst for alkaline seawater oxidation, affords enlarged interlayer spacing of LDH, inhibits chlorine (electro)chemistry, and alleviates local pH drop of the electrode. It only needs an overpotential of 320 mV to reach a current density of 500 mA·cm–2 in 1 M KOH. In contrast to the fast activity decay of NiFe-LDH/CC counterpart during long-term electrolysis, BZ-NiFe-LDH/CC achieves stable 100-h electrolysis at an industrial-level current density of 500 mA·cm–2 in alkaline seawater. Operando Raman spectroscopy studies further identify structural changes of disordered δ (NiIII-O) during the seawater oxidation process.

Highly sensitive flexible pressure sensors play an important role to ensure the safety and friendliness during the human-robot interaction process. Microengineering the active layer has been shown to improve performance of pressure sensors. However, the current structural strategy almost relying on axial compression deformation suffers structural stiffening, and together with the limited area growth efficiency of conformal interface, essentially limiting the maximum sensitivity. Here, inspired by the interface contact behavior of gecko’s feet, we design a slant hierarchical microstructure to act as an electrode contacting with an ionic gel layer, fundamentally eliminating the pressure resistance and maximizing functional interface expansion to achieving ultrasensitive sensitivity. Such a structuring strategy dramatically improves the relative capacitance change both in the low- and high-pressure region, thereby boosting the sensitivity up to 36000 kPa-1 and effective measurement range up to 300 kPa. To verify the advantages of high sensitivity, the sensor is integrated with a soft magnetic robot to demonstrate a biomimetic Venus flytrap. The ability to perceive weak stimuli allows the sensor to be used as a sensory and feedback window, realizing the capture of small live insects and the transportation of fragile objects.

The development of efficient electrochemical seawater splitting catalysts for large-scale hydrogen production is of great importance. In this work, we report an amorphous Co-Mo-B film on Ni foam (Co-Mo-B/NF) via a facile one-step electrodeposition process. Such amorphous Co-Mo-B/NF possesses superior activity with a small overpotential of 199 mV at 100 mA cm−2 for a hydrogen evolution reaction in alkaline seawater. Notably, Co-Mo-B/NF also maintains excellent stability for at least 24 h under alkaline seawater electrolysis.

Abstract Renewable‐electricity‐driven N2 reduction is an attractive approach for ambient NH3 synthesis, but active electrocatalysts are needed to enable the N2 reduction reaction. Monolithic electrodes with active components anchored on conductive supports provide many advantages like structural stability, large surface area, and low electrical resistance. Here, a novel “oxidation‐etching” strategy is proposed to carve the surface of Cu foam into structures of particles, cubes, and sheets for N2 reduction electrocatalysis. The optimal catalyst achieves a Faradic efficiency as high as 18% at −0.35 V vs reversible hydrogen electrode (RHE) and a large NH3 yield of 2.45 × 10−10 mol s−1 cm−1 at −0.40 V vs RHE in 0.1 M HCl. Notably, it also shows superior long‐term electrochemical durability, with the preservation of electro‐activity for at least 20 hours.

Abstract Structure pulverization and poor electrical conductivity of metal dichalcogenides result in serious capacity decay both in lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs). To resolve the above problems, a combination of metal dichalcogenides with conductive scaffolds as high-performance electrode materials has aroused tremendous interest recently. Herein, we synthesize a 3D honeycomb-like rGO anchored with SnS2 quantum dots (3D SnS2 QDs/rGO) composite via spray-drying and sulfidation. The unique 3D-ordered honeycomb-like structure can confine the volume change of SnS2 QDs in the lithiation/delithiation and sodiation/desodiation processes, provide enough space for electrolyte reservoirs, promote the conductivity of the SnS2 QDs, and improve the electron transfer. As a result, the 3D SnS2 QDs/rGO composite electrode delivers a high capacity and long cycling stability (862 mAh/g for LIB at 0.1 A/g after 200 cycles, 233 mAh/g for SIB at 0.5 A/g after 200 cycles). This study provides a feasible synthesis route for preparing 3D-ordered porous networks in varied materials for the development of high-performance LIBs and SIBs in future.

In this work, we study the near-field radiative heat transfer between two suspended sheets of anisotropic 2D materials. It is found that the radiative heat transfer can be enhanced with orders-of-magnitude over the blackbody limit for nanoscale separation. The enhancement is attributed to the excitation of anisotropic and hyperbolic plasmonic modes. Meanwhile, a large thermal modulation effect, depending on the twisted angle of principal axes between the upper and bottom sheets of anisotropic 2D materials, is revealed. The near-field radiative heat transfer for different concentrations of electron is demonstrated and the role of hyperbolic plasmonic modes is analyzed. Our finding of radiative heat transfer between anisotropic 2D materials may find promising applications in thermal nano-devices, such as non-contact thermal modulators, thermal lithography, thermos-photovoltaics, etc.

Cardiac biomarkers (CBs) are substances that appear in the blood when the heart is damaged or stressed. Measurements of the level of CBs can be used in course of diagnostics or monitoring the state of the health of group risk persons. A multi-region bio-analytical system (MRBAS) based on magnetoimpedance (MI) changes was proposed for ultrasensitive simultaneous detection of CBs myoglobin (Mb) and C-reactive protein (CRP). The microfluidic device was designed and developed using standard microfabrication techniques for their usage in different regions, which were pre-modified with specific antibody for specified detection. Mb and CRP antigens labels attached to commercial Dynabeads with selected concentrations were trapped in different detection regions. The MI response of the triple sensitive element was carefully evaluated in initial state and in the presence of biomarkers. The results showed that the MI-based bio-sensing system had high selectivity and sensitivity for detection of CBs. Compared with the control region, ultrasensitive detections of CRP and Mb were accomplished with the detection limits of 1.0 pg/mL and 0.1 pg/mL, respectively. The linear detection range contained low concentration detection area and high concentration detection area, which were 1 pg/mL–10 ng/mL, 10–100 ng/mL for CRP, and 0.1 pg/mL–1 ng/mL, 1 n/mL–80 ng/mL for Mb. The measurement technique presented here provides a new methodology for multi-target biomolecules rapid testing.