Constructing appropriate cocatalysts to modify semiconductors while maintaining tight interface for charge separation facilitation is important for improving photocatalytic hydrogen production. Thus, in this work, C,N-codoped Fe2P/Ni2P (CN/FeNiP) polyhedrons derived from NH2-MIL-101(Fe)/Ni(OH)2 were used as cocatalysts to modify graphitic carbon nitride (g-C3N4) for photocatalytic hydrogen production from water splitting under visible-light irradiation. The highest evolution rate observed over CN/FeNiP/g-C3N4 was 13.81 mmol g−1 h−1 under 1.0 mmol L−1 of Eosin Y (EY) sensitization (compared to 0.196 mmol g−1 h−1 without EY sensitization), which was about 10 and 5 times higher than that of g-C3N4 (1.33 mmol g−1 h−1) and CN/FeP/g-C3N4 (2.73 mmol g−1 h−1). The apparent quantum yield at 420 nm reached 45.8%. A detail analysis of the mechanism revealed that the improved photocatalytic activity can be ascribed to highly efficient spatial separation of photo-induced charges from the excited EY and g-C3N4 to CN/FeNiP with tight interface, staggered band energy between g-C3N4, CN/Fe2P and Ni2P as well as accelerated surface reaction by CN/FeNiP cocatalysts. This work demonstrates that MOF-derived hybrid hollow metal phosphide can be good substitutes for noble metal catalysts for photocatalytic hydrogen production.

NH2-MIL-101(Fe)/Ni(OH)2-derived C,N-codoped Fe2P/Ni2P cocatalyst modified g-C3N4 for enhanced photocatalytic hydrogen evolution from water splitting

Recent advances in application of transition metal phosphides for photocatalytic hydrogen production

MnxCd1-xS solid solution is an emerging semiconductor for photocatalytic water splitting with a tunable bandgap. However, it still leaves much room to improve the photocatalytic activity. Herein, we modified Mn0.5Cd0.5S with noble metal-free NiSe by an in-situ hydrothermal synthesis. The as-obtained NiSe/Mn0.5Cd0.5S nanocomposites exhibited highly efficient photocatalytic H2 production under visible light and the highest hydrogen generation rate reaches 28.08 mmol/h/g, which is higher than that of Mn0.5Cd0.5S (13.71 mmol/h/g) and 1 wt% Pt/Mn0.5Cd0.5S (24.22 mmol/h/g). Through the detailed analyses of UV–vis DRS, photoluminescence (PL) spectra, time-resolved photoluminescence (TRPL) and photoelectrochemical tests, we found the well-matched structure between NiSe and Mn0.5Cd0.5S, which facilitates the charge transfer and prolongs the lifetime of photo-induced electrons, and thus improves photocatalytic activity.

In situ construction of NiSe/Mn0.5Cd0.5S composites for enhanced photocatalytic hydrogen production under visible light

Aqueous Zn‐ion batteries are well regarded among a next‐generation energy‐storage technology due to their low cost and high safety. However, the unstable stripping/plating process leading to severe dendrite growth under high current density and low temperature impede their practical application. Herein, it is demonstrated that the addition of 2‐propanol can regulate the outer solvation shell structure of Zn2+ by replacing water molecules to establish a “eutectic solvation shell”, which provides strong affinity with the Zn (101) crystalline plane and fast desolvation kinetics during the plating process, rendering homogeneous Zn deposition without dendrite formation. As a result, the Zn anode exhibits promising cycle stability over 500 h under an elevated current density of 15 mA cm−2 and high depth of discharge of 51.2%. Furthermore, remarkable electrochemical performance is achieved in a 150 mAh Zn|V2O5 pouch cell over 1000 cycles at low temperature of −20 °C. This work not only offers a new strategy to achieve excellent performance of aqueous Zn‐ion batteries under harsh conditions, but also reveals electrolyte structure designs that can be applied in related energy storage and conversion fields.

Regulation of Outer Solvation Shell Toward Superior Low‐Temperature Aqueous Zinc‐Ion Batteries

Synthesis and photo-catalytic activity of porous g-C3N4: Promotion effect of nitrogen vacancy in H2 evolution and pollutant degradation reactions

Development of highly efficient and low-cost noble metal-free co-catalysts for photocatalytic H2 evolution from water splitting has been aiming at a long-term goal of a renewable hydrogen economy. Herein, a series of novel Mn0.2Cd0.8S/CoP3 composites have been successfully prepared through loading CoP3 nanoparticles on the surface of one dimensional (1D) Mn0.2Cd0.8S nanowires (NWs) by a facile solvothermal method. Under visible light (λ ≥ 420 nm) irradiation, the as-prepared Mn0.2Cd0.8S/CoP3 composite with 2.87 wt% of CoP3 displayed the highest photocatalytic H2 evolution activity with a corresponding H2 evolution rate of 29.53 mmol g−1 h−1 and an apparent quantum yield of 29.2% at 420 nm, which was about 5.02 times higher than that of pure Mn0.2Cd0.8S and 1.79 times than that of Mn0.2Cd0.8S/Pt-1.5 wt%. Moreover, the Mn0.2Cd0.8S/CoP3 composite exhibited excellent photostability. The superior photocatalytic activity of Mn0.2Cd0.8S/CoP3 composite was predominantly attributed to the synergistic effects of highly efficient charge separation efficiency and sufficient active sites for H2 evolution reaction. This work revealed that low-cost CoP3 can replace noble metal Pt as a highly efficient co-catalyst for enhancing the photocatalytic activity of semiconductor materials.

Mn0.2Cd0.8S nanowires modified by CoP3 nanoparticles for highly efficient photocatalytic H2 evolution under visible light irradiation

Iodine has great potential in energy storage, but high solubility of I3- has seriously delayed its promotion. Benefited from abundant active sites and the open channel, two-dimensional coordination supramolecular networks (2D CSNs) is considered to be a candidate for energy storage. Herein, a 2D porphyrin-CSN cathode named Zn-TCPP for aqueous iodine dual-ion battery (DIB) shows an excellent specific capacity of 278 mAh g-1, and a high energy density of 340 Wh kg-1 at 5 A g-1, as well as a durable cycle performance of 5000 cycles and a high Coulombic efficiency of 98%. Molecular orbital theory, UV-vis, Raman spectroscopy and density functional theory (DFT) calculations reveal charge-transfer interaction between the donor of porphyrin nitrogen and the acceptor of I3-, and computational fluid dynamics (CFD) simulations demonstrate the contribution of 2D layered network structure of Zn-TCPP to the penetration of I3-.

A Two-Dimensional Porphyrin Coordination Supramolecular Network Cathode for High-performance Aqueous Dual-Ion Battery.

Facile synthesis Zn-Ni bimetallic MOF with enhanced crystallinity for high power density supercapacitor applications

Iodine is considered to have broad application prospects in the field of electrochemical energy storage. However, the high solubility of I3- severely hampers its practical application, and the lack of research on the anchoring mechanism of I3- has seriously hindered the development of advanced cathode materials for iodine batteries. Herein, based on the molecular orbital theory, we studied the charge-transfer interaction between the acceptor of I3- with a σ* empty antibonding orbital and the donor of pyrimidine nitrogen with lone-pair electrons, which is proved by the results of UV-vis absorption spectroscopy, Raman spectroscopy, and density functional theory (DFT) calculations. The prepared dual-ion battery (DIB) exhibits a high voltage platform of 1.2 V, a remarkable discharge-specific capacity of up to 207 mAh g-1, and an energy density of 233 Wh kg-1 at a current density of 5 A g-1, as well as outstanding cycle stability (operating stably for 5000 cycles) with a high Coulombic efficiency of 97%, demonstrating excellent electrochemical performance and a promising prospect in stationary energy storage.

Anchoring I3- via Charge-Transfer Interaction by a Coordination Supramolecular Network Cathode for a High-Performance Aqueous Dual-Ion Battery.

A scalable manufacturing protocol is developed to prepare polymer-based solvent-free all-solid flexible energy storage devices based on a two-roll mill and adapted rubber mixing technology. The as-prepared solid polymer electrolytes (SPEs) consisting of commercial poly(methyl methacrylate)-grafted natural rubber (MG30) and lithium bis(trifluoromethanesulfonyl)imide achieve a superior ionic conductivity of 2.7 × 10-3 S cm-1 at 30 °C. The superior ionic conductivity is attributed to the formation of an ionic cluster network in the composite as proved by small-angle X-ray scattering and infrared spectroscopy measurements. Moreover, the as-prepared SPEs show good mechanical stability over a broad temperature range, that is , a storage modulus above 1 × 104 Pa from 30 to 120 °C as indicated by the rheology data. Furthermore, the SPEs were assembled with the carbon black-filled MG30 (i.e., MG30C) electrode into a flexible supercapacitor cell, which had a wide voltage window of 3.5 V, good energy density of 28.4 μW h·cm-2 at 160 °C, and good temperature tolerance up to 160 °C. This scaling-up manufacture strategy shows tremendous potential to the advancing of SPEs in applications of flexible energy storage device.

Scalable Manufacturing of Solid Polymer Electrolytes with Superior Room-Temperature Ionic Conductivity.

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