Qipeng Lu (鲁启鹏)

Constructing amorphous/intermetallic (A/IMC) heterophase structures by breaking the highly ordered IMC phase with disordered amorphous phase is an effective way to improve the electrocatalytic performance of noble metal‐based IMC electrocatalysts because of the optimized electronic structure and abundant heterophase boundaries as active sites. In this study, we report the synthesis of ultrathin A/IMC PtPbBi nanosheets (NSs) for boosting hydrogen evolution reaction (HER) and alcohol oxidation reactions. The resulting A/IMC PtPbBi NSs exhibit a remarkably low overpotential of only 25 mV at 10 mA cm‐2 for the HER in an acidic electrolyte, together with outstanding stability for 100 h. In addition, the PtPbBi NSs show high mass activities for methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR), which are 13.2 and 14.5 times higher than those of commercial Pt/C, respectively. Density …

The electrocatalytic nitrate reduction reaction (NO3RR) holds tremendous potential for remediating NO3− pollution in groundwater and obtaining clean ammonia (NH3). However, the currently reported NO3RR catalysts face challenges in achieving high conversion efficiency at low NO3− concentrations due to sluggish reaction kinetics. Herein, we present a highly efficient Mott–Schottky electrocatalyst, composed of an amorphous Co–B nanochain embedded in amorphous CoOx nanosheets (Co–B@CoOx). In 100 ppm NO3−–N, the Co–B@CoOx catalyst exhibits remarkable performance, achieving over 95% NO3− removal within 40 min at −0.90 V vs. reversible hydrogen electrode and nearly 100% NH3 selectivity at −0.80 V, surpassing the performance of both Co–B and CoOx catalysts. Furthermore, Co–B@CoOx demonstrates an ultra-low energy consumption of 0.39 kW h molNO3−1, establishing it as one of the …

Bacterial infections pose a huge threat to human health due to the inevitable emergency of drug resistance. Metal-organic frameworks (MOFs) consisting of metal ions and organic linkers, as emerging efficient antibacterial material, have the merits of structural flexibility and adjustable physicochemical property. With assistance of photosensitive agents as organic linkers, MOFs have great potential in antibacterial application through photocatalytic therapy by the generation of reactive oxygen species (ROS). However, the limited light use efficiency and short lifespan of ROS are two obstacles for their applications. Inspired by the semiconductor heterostructure in photocatalysis, we rationally design and precisely synthesize MOFs based heterostructures, in which the TiO2 nanoclusters are filled into the pores of Cu-TCPP nanosheets (i.e. TiO2 NCs@Cu-TCPP HSs). And the composite materials possess three …

Metastable‐phase intermetallic compounds (IMCs) provide great flexibility to modify the electronic structure and surface coordination environment of metallic catalysts for various reactions. However, the synthesis of metastable‐phase IMCs with high catalytic performance remains a great challenge due to their thermodynamically unstable nature. Here, a wet‐chemical epitaxial growth strategy to synthesize metastable‐phase Pd‐Bi intermetallic nanocrystals (NCs) is reported. β‐Pd3Bi and γ‐Pd5Bi3 intermetallic NCs are epitaxially grown on the templates of face‐centered cubic Pd3Pb nanocubes and hexagonal close‐packed PtBi nanoplates, achieving Pd3Pb@Pd3Bi and PtBi@Pd5Bi3 core–shell NCs, respectively. The obtained Pd3Pb@Pd3Bi NCs possess a mass activity and specific activity of 8.52 A mg−1Pd and 11.59 mA cm−2 for ethanol oxidation reaction, which is 7.5 and 3.6 times as high as those of …

Iridium (Ir) is an efficient catalyst for overall water splitting, yet its widespread utilization is hampered by the substantial cost and limited stability. Alloying Ir with heteroatoms can optimize the electronic structure of the catalyst and reduce the required amount of Ir. Compared to solid solution alloys, Ir‐based intermetallic compounds (IMCs) with ordered and stronger Ir‐heteroatom bonds exhibit superior catalytic activity and durability. Hence, adjusting the crystal structure of Ir‐based IMCs is expected to further optimize the configurations of catalytic active sites with minimal usage of Ir. Here, IrIn2 IMCs with unconventional face‐centered orthorhombic structure are synthesized by a high‐temperature annealing reduction method, in which the atomic percentage of Ir is only 33%. The calculation results show that the d‐band center of IrIn2 is shifted upward compared to metallic Ir, resulting in enhanced adsorption with …

As the global energy crisis intensifies, phase change materials (PCMs) for energy storage have attracted increasing attention in thermal energy storage and thermal management fields. However, due to the lack of an effective thermally conductive network inside, traditional PCMs generally exhibit low thermal conductivity, seriously hampering their practical applications. In this study, vertically aligned AlN skeletons were rationally constructed by freezing casting combined with an in situ carbothermal reduction method and further used as reinforcements to enhance the thermal conductivity of stearic acid (SA)-based PCMs. Benefiting from fast heat transfer channels constructed by the tightly oriented arrangement of AlN particles, the AlN/SA PCMs achieved a highest thermal conductivity of ∼5.74 W m−1 K−1 at a 47.9 vol% filling fraction, exhibiting a thermal conductivity enhancement of 2633.33% compared with that of …

Electrocatalytic nitrate (NO3-) reduction reaction (NO3RR) holds great potential for the conversion of NO3-contaminants into valuable ammonia in a sustainable method. Unfortunately, the non-equilibrium adsorption of intermediates and sluggish multi-electron transfer have detrimental impacts on the electrocatalytic performance of the NO3RR, posing obstacles to its practical application. Herein, we initially screen the adsorption energies of three key intermediates, ie,* NO3,* NO and* H2O, along with the d-band centers on 21 types of transition metals (IIIV and IB)-Sb/Bi based intermetallic compounds (IMCs) as electrocatalysts. The results reveal that hexagonal CoSb IMCs possess the optimal adsorption equilibrium for key intermediates, and exhibit outstanding electrocatalytic NO3RR performance with Faradaic efficiency of 96.3%, NH3 selectivity of 89.1% and excellent stability, surpassing the majority of recently reported NO3RR electrocatalysts. Moreover, the integration of CoSb IMCs/C into a novel Zn-NO3-battery results in a high power density of 11.88 mW cm-2.

Gallium (Ga) with a low melting point can serve as a unique metallic solvent in the synthesis of intermetallic compounds (IMCs). The negative formation enthalpy of Ga-based IMCs endows them with high catalytic stability. Meanwhile, their tunable crystal structures offer the possibility to tailor the configurations of active sites to meet the requirements for specific catalytic applications. Herein, we present a general approach for the synthesis of a range of Ga-based IMCs. The prepared body-centered cubic (bcc) CoGa IMCs are uniformly dispersed on the nitrogen-doped reduced graphene oxide substrate (denoted as CoGa/NG) and deliver outstanding nitrate reduction reaction (NO3RR) performance, which are further used in the highly efficient rechargeable Zn-NO3-battery. Operando studies and theoretical simulations demonstrate that the electron-rich environments around the Co atoms enhance the adsorption strength of* NO3 intermediate and simultaneously suppress the direct dimerization of* H to H2, thus improving the NO3RR activity and selectivity.

The development of electronic devices towards miniaturization and integration has put forward higher requirements for polymer-based composites with high thermal conductivity (TC). Aluminum nitride (AlN) is one of the most promising fillers thanks to its high TC (∼320 W m−1 K−1) and outstanding physicochemical properties. However, the traditional composites filled with randomly dispersed AlN particles generally require extremely high filling fraction to enhance the TC, leading to increased production cost and degraded mechanical performance. To address this issue, an innovative strategy combining freezing casting and in-situ reaction process was proposed to directly construct vertically aligned AlN skeletons, which was further used as reinforcements to enhance the TC of epoxy (EP) composites. The close arrangement of AlN particles along the vertical direction was not only beneficial for enhancing the TC …

As a key structural parameter, phase depicts the arrangement of atoms in materials. Normally, a nanomaterial exists in its thermodynamically stable crystal phase. With the development of nanotechnology, nanomaterials with unconventional crystal phases, which rarely exist in their bulk counterparts, or amorphous phase have been prepared using carefully controlled reaction conditions. Together these methods are beginning to enable phase engineering of nanomaterials (PEN), i.e., the synthesis of nanomaterials with unconventional phases and the transformation between different phases, to obtain desired properties and functions. This Review summarizes the research progress in the field of PEN. First, we present representative strategies for the direct synthesis of unconventional phases and modulation of phase transformation in diverse kinds of nanomaterials. We cover the synthesis of nanomaterials ranging …

Development of suitable colloidal photocatalysts with excellent photocatalytic performance under visible light is essential for indoor environmental remediation. In this study, colloidal Cu-doped TiO2 (Cu-TiO2) nanocrystals containing oxygen vacancies (OVs) were synthesized by a facile sol-hydrothermal method and their photocatalytic performances for benzene degradation and antibacterial were investigated. Characterization results revealed that the doping of Cu induced grain size reduction and bandgap narrowing of TiO2 nanocrystals, as well as the formation of abundant OVs in the TiO2 crystal structure, resulting in enhanced light absorption capacity and charge carrier separation efficiency. The optimized colloidal Cu-TiO2 nanocrystals could achieve a maximum degradation rate constant of 0.364 h−1 for the photocatalytic degradation of benzene and a high antibacterial rate of more than 99.99% against both …

A kind of two-dimensional (2D) metal-organic framework (MOF) material, Cu-meso-tetrakis (4-carboxyphenyl) porphine (Cu-TCPP) nanosheets with wrinkled and flat morphologies are used as building blocks to assemble membranes by vacuum filtration (VF) and electrophoretic deposition (EPD) as energy-efficient nanofiltration (NF) membranes to remove dyes from water. Since the nanosheets with wrinkled structure can provide additional water transport channels, thereby increasing the water permeance, in the premise of a high rejection (> 97.0%) for the dye brilliant blue G (BBG) (1.60 nm × 1.90 nm), the water permeance of the membrane assembled by the wrinkled nanosheets (∼ 1170 nm) is about 4 times that of the membrane assembled by the flat nanosheets (∼ 530 nm), reaching 16.39 L·m−2·h−1·bar−1. Additionally, the use of the relatively flat nanosheets and the membrane preparation method of …

Industrial electrocatalytic hydrogen production puts forward high requirements for catalysts. Compared to the traditional disordered alloy electrocatalysts, intermetallic compounds (IMCs) with ordered atomic arrangement exhibit higher mixing enthalpy and stronger atomic interactions, which greatly improves their catalytic performance and structural stability. Herein, we rationally design and precisely prepare ordered RuGa IMCs with the body-centered cubic structure on N-doped reduced graphene oxide supports (RuGa/N-rGO), which exhibit remarkable HER activities in both acidic and alkaline electrolytes. Notably, the obtained electrocatalyst requires extremely low overpotentials of 105 and 156 mV to deliver 500 and 1000 mA cm−2, respectively, along with high stability over 100 hours continuously running at the overpotential of 100 mV in alkaline electrolyte. Experimental characterizations and theoretical …

In this study, one-dimensional photonic crystal (1DPC) chlorobenzene sensors assembled by ZIF-8, GO, and TiO2 were proposed. The optical properties of 1DPC based on ZIF-8, GO, and TiO2 were studied by varying the number of periods, and the optimized structure of 1DPC based on ZIF-8, TiO2, and GO was to be 2-period. In comparison to the ZIF-8/TiO2 1DPC sensor, the fabricated ZIF-8/GO 1DPC sensor showed better optical sensing properties of chlorobenzene vapor, which showed stronger selectivity, higher sensitivity, and lower limit of detection (0.55 ppm). The sensitivity of the ZIF-8/GO 1D PC sensor (0.18 nm/ppm) is almost 3 times higher than that of ZIF-8/TiO2 1D PC sensor (0.05 nm/ppm) at 0–100 ppm concentration of chlorobenzene vapor. The relationship between the reflected spectra shifts and chlorobenzene of low concentrations was presented to be high linearity. Moreover, the ZIF-8/GO 1DPC …

The direct electrochemical nitric oxide reduction reaction (NORR) is an attractive technique for converting NO into NH3 with low power consumption under ambient conditions. Optimizing the electronic structure of the active sites can greatly improve the performance of electrocatalysts. Herein, we prepare body‐centered cubic RuGa intermetallic compounds (i.e., bcc RuGa IMCs) via a substrate‐anchored thermal annealing method. The electrocatalyst exhibits a remarkable NH4+ yield rate of 320.6 μmol h−1 mg−1Ru with the corresponding Faradaic efficiency of 72.3 % at very low potential of −0.2 V vs. reversible hydrogen electrode (RHE) in neutral media. Theoretical calculations reveal that the electron‐rich Ru atoms in bcc RuGa IMCs facilitate the adsorption and activation of *HNO intermediate. Hence, the energy barrier of the potential‐determining step in NORR could be greatly reduced.

Metal–organic frameworks (MOFs), as a class of semiconductor-like materials, are widely used in photocatalysis. However, the limited visible light absorption and poor charge separation efficiency are the main challenges restricting their photocatalytic performance. Herein, the type II heterojunction MIL-68(In)@ZIS was successfully fabricated by in situ growth of ZnIn2S4 (ZIS) on the surface of a representative MOF, i.e. MIL-68(In). After composition optimization, MIL-68(In)-20@ZIS shows an extraordinary photocatalytic hydrogen production efficiency of 9.09 mmol g−1 h−1 and good photochemical stability, which far exceeds those of most photocatalysts. The hierarchical loose structure of MIL-68(In)-20@ZIS is conducive to the adsorption of reactants and mass transfer. Meanwhile, a large number of tight 2D contact interfaces significantly reduce the obstruction of charge transfer, paving the way for high-perform …

Rhodium (Rh) has received widespread attention in fundamental catalytic research and numerous industrial catalytic applications. Compared to homogeneous catalysts, Rh-based nanomaterials as heterogeneous catalysts are much easier to separate and collect after usage, making them more suitable for commercial use. To this purpose, there has been a constant demand in constructing stable and highly active Rh-based nanomaterials. In contrast to Rh-based solid solutions with a random distribution of metallic atoms in the lattice, Rh-based intermetallic compounds (IMCs) with a fixed stoichiometric ratio and an ordered atomic arrangement can ensure the homogenous distribution of active sites and structural stability in the catalytic process. In this review, we concentrate on the fabrication of Rh-based IMCs for catalytic applications. Various synthetic methods and protocols for the controlled preparation of Rh …

1, 导读: 二维贵金属基金属间化合物 (IMC) 催化剂已在能源催化应用中展现出广阔的前景. 本综述总结了二维贵金属基 IMC 的合成及其在电催化应用的最新研究进展, 提出了该领域存在的主要挑战和未来研究方向.

Electrochemical nitrate (NO3−) reduction reaction (NO3RR) possesses two-pronged properties for sustainable ammonia (NH3) synthesis and mitigating NO3− contamination in water. However, the sluggish kinetics for the direct eight-electron NO3−-to-NH3 conversion makes a formidable challenge to develop efficient electrocatalysts. Herein, we report a heterostructure of Co3O4 nanosheets decorated TiO2 nanobelt array on titanium plate (Co3O4@TiO2/TP) as an efficient NO3RR electrocatalyst. Both experimental and density theory calculations reveal that the heterostructure of Co3O4@TiO2 establishes a built-in electric field which can optimize the electron migration kinetics, as well as facilitate the adsorption and fixation of NO3− on the electrode surface, ensuring the selectivity to NH3. As expected, the designed Co3O4@TiO2/TP exhibits a remarkable Faradaic efficiency of 93.1 % and a remarkable NH3 yield …

Abstract Electrochemical nitrite (N O 2−) reduction can produce value-added ammonia (NH 3) and simultaneously eliminate N O 2− pollutants in surface water and underground water. However, the complicated six-electron N O 2− reduction reaction (NO 2 RR) needs efficient electrocatalysts with high selectivity. Herein, we report that Ni-doped TiO 2 nanoribbon array on titanium plate (Ni–TiO 2/TP) acts as a high-active NO 2 RR electrocatalyst with a large NH 3 yield of 380.27 μmol/h/cm 2 and a high Faradaic efficiency of 94.89%, superior to TiO 2/TP. Density functional theory calculations reveal that Ni doping can enhance the intrinsic electrical conductivity and optimize the adsorptive free energy of intermediates for high N O 2−-to-NH 3 selectivity.