APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Haimin Liu,Mengmeng Jin,Da Zhan,Jinming Wang,Xiaoyi Cai,Yongting Qiu,Linfei Lai
Structure modulation of transition metal phosphides at the atomic scale can significantly modify their catalytic properties. Herein, stacking faults abundant Ni 2 P/Co 2 P electrocatalysts with outstanding bifunctional oxygen evolution and hydrogen evolution property have been prepared. The stacking faults are formed by slow dissolution of Ni substrate by Mo 6+ and further redeposition of Ni 2+ during the growth of Co(OH)F crystals. Unprecedentedly, the distinct mechanistic etching-redeposition pathway dictated by the stacking faults, heterostructures and crystal lattice deformation leads to lattice expansion of Co 2 P and enables preferred reactants adsorption. Electrolysis cell employing Ni 2 P/Co 2 P electrocatalysts as a bifunctional catalyst for both the cathode and the anode delivers a current density of 10 mA cm −2 at a cell voltage of 1.57 V, which is comparable to the integrated Pt/C and IrO 2 counterparts. The exceptional electrocatalytic performance of Co 2 P/Ni 2 P-x%Mo indicates the redeposition mechanism a new methodology to modulate the structure and surface reactivity of electrocatalysts.
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2022
·Vol. 33
·期 34
·25768-25786
·
IF 2.779
Liang Ying,Xu Huimin,Zhang Zhen,Fang Bin
Transition metal cobalt–nickel hydroxides have been widely studied as electrode materials for hybrid supercapacitors (HSCs) due to their unique active component properties. Nevertheless, the influencing factors and optimization of their electrochemical performances are still being studied and discussed. In this paper, Co–Ni layered double hydroxide (LDH) porous structure assembled from nanosheets was formed directly on stainless steel wire mesh (SS) by potentiostatic deposition. The bimetallic synergistic effect and porous structure of Co–Ni LDHs are favorable to their electrochemical performances. The Co 0.5 Ni 0.5 (OH) 2 −SS (nominal composition) electrode has the optimal Co:Ni molar ratio, and its specific capacity values are 474.2 − 320.1 C g −1 at different current densities (1–10 A g −1 ) in 1 M KOH electrolyte. In addition, the concentration of KOH electrolyte also plays an important role on the electrochemical mechanism and performances. Compared with 6 M KOH electrolyte, lower concentration (1 and 3 M) is much more conductive to the microstructural stability and electrochemical behaviors of Co 0.5 Ni 0.5 (OH) 2 −SS electrode. Moreover, the fabricated Co 0.5 Ni 0.5 (OH) 2 −SS//AC−SS HSC device exhibits a good cycling stability, and the maximum energy density is about 10.9 Wh kg −1 at 548.0 W kg −1 .
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Journal of the American Chemical Society
·
2020
·
IF 14.612
Kaihui Mao,Jinlei Zhang,Zijing Guo,Lizhe Liu,He Ma,Yiying Chin,Hongji Lin,Songsong Bao,Hangqing Xie,Run Yang,Zhaoyang Jing,Jiancang Shen,Guoliang Yuan,Jian Chen,Peiheng Wu,Xinglong Wu
Layered metal–organic structures (LMOSs) as magnetoelectric (ME) multiferroics have been of great importance for realizing new functional devices in nanoelectronics. Until now, however, achieving such room-temperature and single-phase ME multiferroics in LMOSs have proven challenging due to low transition temperature, poor spontaneous polarization, and weak ME coupling effect. Here, we demonstrate the construction of a LMOS in which four Ni-centered {NiN2O4} octahedra form in layer with asymmetric distortions using the coordination bonds between diphenylalanine molecules and transition metal Ni(II). Near room-temperature (283 K) ferroelectricity and ferromagnetism are observed to be both spontaneous and hysteretic. Particularly, the multiferroic LMOS exhibits strong magnetic-field-dependent ME polarization with low-magnetic-field control. The change in ME polarization with increasing applied magnetic field μ0H from 0 to 2 T decreases linearly from 0.041 to 0.011 μC/cm2 at the strongest ME coupling temperature of 251 K. The magnetic domains can be manipulated directly by applied electric field at 283 K. The asymmetrical distortion of Ni-centered octahedron in layer spurs electric polarization and ME effect and reduces spin frustration in the octahedral geometry due to spin-charge-orbital coupling. Our results represent an important step toward the production of room-temperature single-phase organic ME multiferroics.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Jun-Ke Liu,Zu-Wei Yin,Wei-Chen Zheng,Jing Zhang,Sai-Sai Deng,Zhen Wang,Li Deng,Shi-Jun Xie,Zong-Kui Liu,Maxim Avdeev,Fengjin Qu,Wang Hay Kan,Yao Zhou,Jun-Tao Li
A Ni-rich layered oxide, one promising cathode for lithium-ion batteries (LIBs), exhibits the advantages of low cost and high capacity but suffers from rapid capacity loss due to bulk structural instability and surface side reactions. Herein, a simple synchronous dual-modification strategy with Zr4+ doping and CeO2 nanowelding is proposed to address such issues. Utilizing the migration energy difference of Zr and Ce ions in layered structures, one-step high-temperature sintering of LiNi0.8Co0.1Mn0.1O2 particles with Zr and Ce nitrate distributions enables simultaneous doping of Zr ions in the bulk and CeO2 surface modification. Therein, Zr ions in the bulk occupying the Li sites can improve the Li+ diffusion rate and stabilize the crystal structure, while CeO2 on the surface provides nanowelding between the grain boundaries and resistance to electrolyte erosion. Theoretical calculations and a series of structure/composition characterizations (i.e., neutron scattering, in situ X-ray diffraction, etc.) validated the proposed strategy and its role in stabilizing the Ni-rich cathodes. The synergistic effect of Zr4+ doping and CeO2 nanowelding enables an impressive initial capacity of 187.2 mAh g–1 (2.7–4.3 V vs Li/Li+) with 86.1% retention after 200 cycles at 1 C and rate capabilities of 146.6 and 127.3 mAh g–1 at 5 and 10 C, respectively. Upon increasing the testing temperature to 60 °C, the dual-modified Ni-rich cathode exhibits an initial discharge capacity of 203.5 mAh g–1 with a good retention of 80.8% after 100 cycles at 0.5 C. The present strategy utilizing the migration energy difference of metal ions to achieve synchronous bulk doping and surface modification will offer fresh insights to stabilize layered cathode materials for LIBs, which can be widely used in other kinds of batteries with various cathode materials.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Yi Zhou,Wenbiao Zhang,Jialai Hu,Dan Li,Xing Yin,Qingsheng Gao
Unraveling structure-related reconstruction during oxygen evolution reaction (OER) and its correlation with intrinsic electrocatalytic activity is of great significance for designing better catalysts but unfortunately remains elusive. Herein, ultrathin Ni-Fe layered-double-hydroxides (LDH) with inherent oxygen vacancies (VO) are successfully fabricated via coprecipitation under a controlled manner, which accomplish a quite low overpotential of 230 mV at 10 mA cm–2 in 1.0 M KOH and perform among the best of recently reported nonprecious electrocatalysts. During the OER, inherent VO is experimentally and theoretically evidenced to boost surface reconstruction and the operando formation of p–n interfaces (i.e., γ-Ni-Fe LDH/α-Ni-Fe LDH) via deprotonation. On such reconstructed interfaces, the VO in both surface γ-Ni-Fe LDH and bulk α-Ni-Fe LDH can alter the electron densities of metal sites and subsequently optimize the free energies of a multistep OER pathway, which accounts for the boosted OER activity and, more importantly, identifies the correlation of electrocatalysis with both the catalyst surface and bulk.
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高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Guangchang Yang,Shenglong Yang,Feiyan Lai,Chunlei Tan,Jia Qiao,Hongqiang Wang,Qianqian Jin,Xiaohui Zhang
Current research has found the amorphous/crystal interface has some unexpected electrochemical behaviors. This work designed a surface modification strategy using NaBH4 to induce in situ conversion of the surface structure of Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) into TM-B-O amorphous interface layer. Oxidizing the surface from transition metals (TM) with high valence and reductive BH4– in a weak polar medium of ethanol results in an easy redox reacton. A TM-B-O amorphous structure is formed on NCM811 surface. The action of reactive wetting ensures a complete and uniform structure evolution of the surface crystals. The complete coverage protects the outer crystal and the heterogeneous interface impedance between the modified layer and bulk is reduced. More importantly, this amorphous interface layer through in situ conversion enhances the heterogeneous link at interface and its own structural stability. The modified NCM811 (TB2@NCM) treated with 1 wt % NaBH4 shows excellent electrochemical performance, especially cyclic stability. At a high cutoff voltage of 4.5 V, the capacity retention was 72.5% at 1 C after 500 cycles. The electrode achieves 173.7 mAh·g–1 at 10 C. This work creates a modifying strategy with potential application prospect due to simple technology with low-cost raw material under mild operating conditions.
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JOURNAL OF SOLID STATE CHEMISTRY
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2024
·
IF 3.2
Qianni Bian,Shutao Li,Ruyang Shen,Shiqi Shen,Ziheng Wen,Xu Jiang,Faliang Gou
A mesoporous silica-supported Ni–Co composite metal oxide has been synthesized and applied as an effective heterogeneous catalyst for the selective catalytic oxidation of benzyl alcohols . Various characterization methods were employed to confirm the successful synthesis of the catalysts and their nanostructure . The catalytic performances of these catalysts in the selective oxidation of substituted benzyl alcohols to aromatic aldehydes were systematically investigated using molecular oxygen from the air as the oxidant under atmospheric pressure. The NiCo@SBA-15 catalyst exhibited remarkable performance, achieving nearly 98 % conversion and almost complete selectivity at a temperature of 120 °C for 10 h, operating at 1 atm of air pressure. This catalytic performance can be attributed to the synergistic effect between Ni and Co ions , resulting in the generation of new surface-active sites in the catalyst. The catalyst also demonstrated favorable applicability and universality. Moreover, A plausible catalytic mechanism has been proposed involving the synergistic effect between bimetal species and oxygen vacancy .
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Rushuo Li,Tao Ban,Danfeng Zhao,Fajie Hu,Jing Lin,Xiubing Huang,Zhiping Tao,Ge Wang
Defect engineering improves the catalytic performance of metal-organic frameworks (MOFs) loaded metal nanoparticles (MNPs@MOFs), but there is still a challenge in defining the structure-activity relationships. Herein, the content of linker-missing defects in UiO-66(Ce) was systematically regulated via formic acid as the modulators, and defective UiO-66(Ce) loaded Ni nanoparticles (NPs) were constructed for dicyclopentadiene (DCPD) hydrogenation. The fine regulation of defect engineering and reduction conditions affected the structure properties of UiO-66(Ce) and the electronic metal-support interaction between MOFs and Ni NPs, thereby optimizing the microenvironment and electronic state of Ni NPs. The optimized U(Ce)-40eq with suitable defects, small size and structure stability effectively promoted the production of highly dispersed abundant electron-deficient Ni 0 active sites, enhancing the adsorption and activation of H 2 and C=C bonds, especially accelerating the rate-determining step. Therefore, U(Ce)-40eq loaded 5 wt% Ni NPs achieved DCPD saturated hydrogenation to tetrahydrodicyclopentadiene (70 °C, 2 MPa, 90 min), superior to most high-loading Ni-based catalysts. This work reveals the synergistic mechanism of MOFs defect engineering and electronic structure of Ni NPs, providing effective guidance for the precise preparation of highly efficient and stable MNPs@MOFs heterogeneous catalysts.
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高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 5
·1-19
·
IF 2.4
Hu Xinyin,Xiao Guoqing,Chen Chunlin,Chen Chunyan,Zeng Xiang,Li Ruili,Yang Zhengwei
Recently, several emerging pollutants have caused increasing damage to aquatic ecosystems. Reducing antibiotic concentrations in water by visible light is one of the most promising strategies for sustainable development. Here, a Bi 2 S 3 /CeO 2 /Ni(OH) 2 Z-scheme heterojunction photocatalyst was prepared by the hydrothermal method, which could effectively utilize free radicals to degrade tetracycline. Ni(OH) 2 was used for co-catalysing in photodegradation experiments to improve electron transfer and enhance photocatalytic performance. The degradation rate of the Z-scheme heterojunction photocatalyst for 20 mg/L TC was 91.35% after reacting 60 min under visible light irradiation. Besides, it also investigated such operational parameters influencing the photocatalytic reaction as catalyst dosage, initial concentration of tetracycline hydrochloride (TC), and solution pH. Studies using free radical scavenging experiments and electron spin resonance (ESR) measurements demonstrated that hydroxyl radicals (·OH) and superoxide radicals (·O 2 − ) both contributed to the photodegradation of TC. Finally, with high-performance liquid chromatography-mass spectrometry (LC-MS), potential degradation pathways of the intermediate products were logically inferred as well as the photocatalytic mechanism. The experimental results surface that the prepared Z-scheme heterojunction photocatalyst Bi 2 S 3 /CeO 2 /Ni(OH) 2 exhibits superior photocatalytic performance, offering a novel approach to addressing TC contamination in environmental settings. Graphical
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Xu Guangyuan,Peng Xingjie,Wu Chuanqiang,Xi Shibo,Xiang Huixin,Feng Lei,Liu Zhendong,Duan Yi,Gan Lijin,Chen Si,Kong Yuan,Ma Yanzhe,Nie Fujing,Zhao Jie,Hai Xiao,Wei Wei,Zhou Meng,Wang Tianfu,Yao Chuanhao,Zhou Wu,Yan Huan
CO 2 electroreduction to CO promises to give an efficient strategy for CO 2 fixation and transformation. However, current reported active sites fail to deliver sufficient activity with high CO Faradic efficiency (FEco) over a wide range of potential. Here, we show a general synthetic protocol to fabricate a batch of highly pure and active NiN 2 catalysts with precise engineering of the uniform-large ( UL ) vacancy around the active sites, which is accomplished through the ‘pre-deposition + pyrolysis’ of various atomically precise Ni clusters (Ni n ) and in-situ etching of the support by the ‘nano bomb’ (sulfur-ligand in the clusters). The NiN 2 sites with UL vacancies could achieve a high turnover frequency (TOF) of 350000 h −1 with ~100% FEco in a wide potential range of 1500 mV. In-situ infrared spectra and theoretical calculations reveal that a highly pure NiN 2 site with UL vacancy contributes to this remarkable catalytic performance compared to the counterparts. This general synthetic strategy enables us to simultaneously engineer active sites and surrounding vacancies with the employment of atomically precise metal clusters, thereby enhancing catalytic performance for other specific reactions.
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DOI
PubMed
高影响因子
Scientific Reports
·
2025
·Vol. 15
·期 1
·1-14
·
IF 3.9
Liu Liming,Lian Hongxia,Deng Heming,Zhang Weixin
Challenges associated with the cathode material of Lithium–oxygen (Li–O 2 ) battery, particularly the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction, as well as the accumulation of discharge product Li 2 O 2 , have hindered its further advancement. Here, an in-situ synthesis strategy was adopted to load a bimetallic Ni–Co metal–organic framework (Ni/Co-MOF) onto MXene (Ti 3 C 2 ) layers. Subsequently, a free-standing and flexible Ni/Co-MOF@Ti 3 C 2 hybrid membrane is prepared via a layer-by-layer self-assembly method, specifically designed for efficient ORR and as a cathode for Li–O 2 batteries. The Ni/Co-MOF@Ti 3 C 2 hybrid membrane integrates the high conductivity, unique two-dimensional layered structure, and excellent mechanical properties of Ti 3 C 2 with the bimetallic active sites of Ni/Co-MOF, exhibiting remarkable ORR catalytic activity in an O 2 -saturated 1 M LiTFSI electrolyte. The structural characteristics of the hybrid membrane provide smoother expansion pathways for Li + and O 2 , effectively promoting the deposition and decomposition of Li 2 O 2 . This not only enhances the electrochemical performance of the Li–O 2 battery but also overcomes the inherent limitations of traditional slurry-based cathode preparation methods. Experimental results demonstrate that Li–O 2 batteries utilizing the Ni/Co-MOF@Ti 3 C 2 hybrid membrane as the cathode achieve an ultra-high capacity of 36,125 mAh/g at a current density of 1000 mA/g, while exhibiting excellent cycle stability (271 cycles with a limited capacity of 1000 mAh/g at 1000 mA/g) and outstanding rate performance. The hybrid membrane’s capacity and cycle performance can be further optimized by controlling its thickness. These promising results offer novel insights into the innovative design of air cathodes for metal–air batteries, and the proposed method provides a new route for the manufacture of high-performance battery cathodes.
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PubMed
高影响因子
Separations
·
2024
·Vol. 11
·期 11
·305
·
IF 2.5
Jingmin Duan,Yafei Zhao,Zhuhe Zhai,Shengqiang Chen,Bing Zhang
Efficient and low-cost nanocatalysts are extremely desirable for the catalytic reduction of 4-nitrophenol (4-NP). A smaller nanocatalyst particle size and stronger support effect can significantly enhance the catalytic performance. Naturally occurring halloysite nanotubes (HNTs) are promising alternative supports for fine metal nanoparticles, but the smooth surface and single type of functional groups on HNTs are usually unfavorable for the anchoring of metal ions. Herein, we modified HNTs using a mild and controllable molten salt etching method to create a rough surface (rHNTs), followed by loading Pt–Ni alloys to prepare Pt–Ni/rHNTs for the catalytic reduction of 4-NP. The results demonstrate that ultrafine Pt–Ni alloy nanoparticles with a diameter of 1.60 nm are uniformly dispersed on the rough surface of rHNTs. The particle size and catalytic performance can be tuned by adjusting the loading amount of Pt–Ni. The optimized Pt–Ni/rHNT (1 wt %) nanocatalyst reveals the smallest Pt–Ni particle size and the highest catalytic rate of 0.1953 min−1, which exceeds many Pt–Ni-based catalysts in previous reports. This work offers an ingenious idea for the mild surface modification of HNTs and a brilliant perspective for the rational design of inexpensive 4-NP reduction nanocatalysts.
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