JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
·
IF 4.464
Ya Liu,Wenzhu Tang,Gaowei Zhang,Wenhao Chen,Qingze Chen,Chunlin Xiao,Shenghui Xie,Yejun Qiu
Developing stable and efficient electrocatalysts for hydrogen evolution reaction is of great significance for the production of clean hydrogen energy from water splitting. In this work, 3D AgNWs@NiMo/PU electrode was obtained by electrodepositing NiMo alloy onto three-dimensional silver nanowires conductive substrate (3D AgNWs/PU) which was uniformly assembled on the surface of the skeleton of a polyurethane sponge (PU). 3D AgNWs/PU provides good electrolyte permeability, rich active site attachment points, good electronic conductivity and electrocatalytic synergy, which greatly improves the catalytic activity. In addition, 3D AgNWs@NiMo/PU electrode does not need to use adhesive in the process of hydrogen evolution, which can improve the hydrogen evolution performance and stability of the electrode. Specifically, the optimized electrode (AgNWs@NiMo/PU-1200 s) exhibits excellent hydrogen evolution performance by achieving a low overpotential of 32 mV (vs. RHE) at a current density of 10 mA cm −2 , with a Tafel slope of 72 mV dec -1 (in 1 M KOH). More interestingly, it also has good stability after 10 h of stability test. Therefore, this study provides a feasible way to develop stable and efficient 3D HER electrocatalysts.
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ACS Catalysis
·
2017
·
IF 10.614
Chaofeng Zhang,Hongji Li,Jianmin Lu,Xiaochen Zhang,Katherine E. MacArthur,Marc Heggen,Feng Wang
For lignin valorization, simultaneously achieving the efficient cleavage of ether bonds and restraining the condensation of the formed fragments represents a challenge thus far. Herein, we report a two-step oxidation–hydrogenation strategy to achieve this goal. In the oxidation step, the O2/NaNO2/DDQ/NHPI system selectively oxidizes CαH–OH to Cα═O within the β-O-4 structure. In the subsequent hydrogenation step, the α-O-4 and the preoxidized β-O-4 structures are further hydrogenated over a NiMo sulfide catalyst, leading to the cleavage of Cβ–OPh and Cα–OPh bonds. Besides the transformation of lignin model compounds, the yield of phenolic monomers from birch wood is up to 32% by using this two-step strategy. The preoxidation of CαH–OH to Cα═O not only weakens the Cβ–OPh ether bond but also avoids the condensation reactions caused by the presence of Cα+ from dehydroxylation of CαH–OH. Furthermore, the NiMo sulfide prefers to catalyze the hydrogenative cleavage of the Cβ–OPh bond connecting with a Cα═O rather than catalyze the hydrogenation of Cα═O back to the original CαH–OH, which further ensures and utilizes the advantages of preoxidation.
研究领域:
化学工程
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生物质转化
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催化反应
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FUEL
·
2025
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IF 7.5
Muhammad Chawla,Xiyue Lu,Mooeez ur Rehman,Fan Sun,Wei Liu,Shengnian Wang,Yongli Ma,Mingyan Liu,Yujun Zhao
It is highly desired to use non-noble metal catalysts for efficiently upgrading biomass into biofuels and value-added products. A series of Ni-Mo bimetallic catalysts were synthesized using hydrothermal method; and employed in the hydrodeoxygenation (HDO) of guaiacol to cyclohexane. The resulting highly dispersed catalyst with an optimal Ni/Mo ratio, Ni 0.75 Mo 0.25 ZrO 2 demonstrated outstanding HDO performance with a 100 % yield of cyclohexane under 250 ℃ and 5 MPa due to the synergistic effect of NiMo alloy and metallic Ni. Further characterization results reveal that enhanced catalytic activity is primarily attributed to the improved dispersion of metal on ZrO 2 support, facilitated by the formation of NiMo alloy. The introduction of Mo into the Ni framework alters the surface structure, breaking up the continuous Ni surface into smaller ensembles. Additionally, the presence of Mo reduces the d-band electron density of Ni, creating an electron deficient Ni-Mo interface that increase the Lewis acid sites. This modification increases the number of available Lewis acid sites, promoting efficient catalytic processes. Furthermore, the altered surface structure enhances the interaction between the oxygen atom and Mo, thereby facilitating the conversion of cyclohexanol to cyclohexane. This catalyst was found also exceptionally efficient in cleaving the α-O-4 and β-O-4 ether linkages in various lignin-derived model compounds. Together with excellent stability and remarkable adaptability, this bimetallic catalyst exhibits promising potential in production of diesel from lignin resources to pave the way for green and sustainable supply of fuels.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2024
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IF 4.4
Xiaohui Yang,Qi Ye,Fei Ge,Minghao Zhou
Lignin, as an important biomass resource, has significant research value in its oxidative cleavage process. Nickel-based metal catalysts could selectively depolymerize lignin. A series of heteropolyacid doped nickel based bimetallic catalysts Ni 4 Mo 1 -MOF-x（x represented heteropolyacid）were prepared by hydrothermal method, which were calcined to catalyze the oxidative cleavage of lignin model compound (2-phenoxy-1-acetophenone). The catalyst Ni 4 Mo 1 -MOF-SiWA-0.1(500) showed the best catalytic performance in methanol solvent under conditions of 160 °C, 4 h, 0.5 MPa oxygen pressure, where the conversion rate was nearly 100 % and the yields of phenol and benzoic acid were 54.5 % and 23.3 %, respectively. The catalysts were well characterized to explore the catalytic performance during the oxidation of lignin dimer. This study could provide some interesting and useful information for the catalytic oxidation of lignin to biomass-derived chemicals.
研究领域:
生物质化学
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催化化学
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FUEL
·
2023
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IF 7.4
Shiyu Wu,Feng Long,Xincheng Cao,Peng Liu,Yanju Lu,Junming Xu
Selective hydrodeoxygenation is the central challenge in converting bio-derived fatty acids into fatty alcohols under mild conditions. Herein, an effective and highly selective carbon-supported NiMo catalyst (NiMo@C) was developed by the thermolysis Ni-based metal–organic frameworks (MOF) impregnated Mo species. At a low temperature of 160 °C, the stearic acid can be efficiently converted into corresponding stearic alcohols over the NiMo@C with about 97% selectivity at 100% reactant conversion, which is superior to the most reported catalysts containing noble catalysts. The excellent catalytic performance of NiMo@C catalyst was mainly attributed to the ordered arrangement of Ni in the MOF and the uniform loading of molybdenum salt, which leads to an ideal distribution of Ni and Mo after pyrolysis of the MOF. The carbon support also prevents the aggregation of metal particles, which promotes the dissociation of hydrogen and enhances the synergy between Ni and Mo sites. More importantly, the synthesized NiMo@C catalyst showed excellent reusability with no loss of activity after 15 consecutive runs due to the stability of the catalyst structure. This provides a useful and simple method for synthesizing highly efficiency and stable NiMo@C bimetallic catalysts, which can facilely and selectively hydrogenate the bio-derived fatty acids to corresponding alcohols under mild conditions.
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NANOTECHNOLOGY
·
2020
·Vol. 31
·期 49
·495404
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IF 3.551
Saman Sajjad,Chao Wang,Xianfu Wang,Tariq Ali,Tao Qian,Chenglin Yan
Due to their good conductivity and catalytic performance, Ni—Mo-based catalysts are well-established for highly effective water splitting. However, the know-how required to fabricate distinct interfaces and electronic structures for metal oxides is still a challenge, and the synergistic effect between metal and metal oxides that enhances electrocatalytic activity is still ambiguous. As described here, by controlling the lithium-induced conversion reaction of metal oxides, metal/metal-oxide composites with plentiful interfaces and prominent electrical interconnections were fabricated, which can boost active sites and accelerate mass transfer during electrocatalytic reactions. As a consequence, the superior catalytic activity of ECT-NiMo/NiMoO4 exhibited a low overpotential of 61 mV at a current density of 10 mA cm−2 for the hydrogen evolution reaction and 331 mV at 100 mA cm−2 for the oxygen evolution reaction. When integrated into a two-electrode system, the ECT-NiMo/NiMoO4 revealed a highly stable and efficient performance in overall water splitting. This work provides a promising approach to enhance the metallicity and electron redistribution of catalysts for numerous water-splitting applications and many other possibilities for energy storage devices.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Wei Liu,Yusen Yang,Lifang Chen,Enze Xu,Jiaming Xu,Song Hong,Xin Zhang,Min Wei
Activation of oxygen-containing functional groups plays a key role in sustainable biomass upgrading and conversion. In this work, a NiMo intermetallic compound (IMC) catalyst was prepared based on layered double hydroxides (LDHs) precursors, which displayed prominent catalytic performance for furfural hydrodeoxygenation (HDO) to 2-methylfuran (2-MF) (yield: 99 %) at a rather low hydrogen pressure (0.1 MPa), significantly superior to NiMo alloy, monometallic Ni and other Ni-based catalysts ever reported. CO-IR, STEM, EXAFS and XANES give direct evidences that the atomically-ordered Ni/Mo sites in NiMo IMC determine the uniform bridging-type adsorption mode of C O bond in furfural whilst adsorption of furan ring is extremely suppressed. In situ FT-IR and DFT calculation further substantiate that ordered Ni-Mo bimetallic sites of IMC, in contrast to the random atomic sequence in NiMo alloy, facilitate the activation and cleavage of C OH bond in the intermediate (furfuryl alcohol, FOL), accounting for the production of 2-MF. This work demonstrates the decisive effect of atomically-ordered active sites in IMC catalyst on activation of oxygen-containing functional groups and product selectivity, which can be extended to catalytic upgrading of biomass-derived platform molecules.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2026
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IF 10.5
Ju-Hua Li,Yong Tian,Jia-Yi Chen,Hong-Kai Guo,Wen-Hao Wang,Yu-Shu Han,He-Xuan Zhang,Xiao-Yu Zhang,Zhong-Li Wang
Citric acid adsorbed CeO 2 forms a uniformly dispersed nanoparticle sol, acting as a special “glue” to uniformly adhere to the surface of the NiMoO 4 precursor. • Under high-temperature reduction, a CeO 2-x modified NiMo alloy with strong interaction is synthesized. • The optimized composite electrocatalyst achieves an overpotential of only 48 mV at 10 mA cm -2 with the stability for over 1,500 h at 500 mA cm -2 . • In situ Raman spectra and DFT calculations indicate that the CeO 2-x /NiMo alloy interface accelerates water dissociation and enhances alkaline HER performance. NiMo alloys are promising non-precious metal electrocatalysts for alkaline hydrogen evolution reaction (HER), however, they suffer from issues such as poor stability due to Mo leaching and insufficient intrinsic activity. In this study, a citric acid (CA) assisted CeO 2-x modification strategy is developed to prepare a CeO 2-x /NiMo alloy composite electrocatalyst with high activity and stability. CA is uniformly adsorbed onto the surface of CeO 2 nanoparticles, and the cross-linked CA network with the CeO 2 particles forms a uniformly dispersed nanoparticle sol, which acts as a special “glue” to uniformly adhere to the surface of the NiMoO 4 precursor, forming a CeO 2 /NiMoO 4 composite precursor. Following high-temperature reduction, a CeO 2-x modified NiMo alloy electrocatalyst is synthesized. Owing to the strong interaction between CeO 2-x and NiMo, the optimized composite electrocatalyst achieves a current density of 10 mA cm -2 at an overpotential of only 48 mV and it maintains high stability for over 1500 h at a current density of 500 mA cm -2 , which is three times longer than that of the unmodified NiMo alloy electrocatalyst, outperforming most reported nickel-molybdenum-based electrocatalysts. In situ Raman spectra and density functional theory calculations indicate that the CeO 2-x /NiMo alloy interface accelerates water dissociation, hydrogen combination and enhances alkaline HER performance. This work provides a new approach for the preparation of highly active and stable nickel-molybdenum-based hydrogen evolution catalysts. A citric acid assisted CeO 2-x modification strategy is developed to prepare a highly-active and stabile CeO 2-x /NiMo alloy electrocatalyst for HER. Download: Download high-res image (267KB) Download: Download full-size image
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NANO
·
2019
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IF 1.293
Wen Yang,Bin Xia,Jiacheng Lu,Peizhi Yang,Xiaobo Chen
Novel hierarchical porous NiMoS 4 microspheres with high electrochemical performance was successfully prepared using a facile one-step hydrothermal method. The dual application of porous NiMoS 4 microspheres in energy harvesting and storage (i.e., dye-sensitized solar cells (DSSCs) and supercapacitors (SCs), respectively) is explored. In contrast to NiS 2 nanosheets, MoS 2 nanosheets and Pt counter electrodes (CEs), the NiMoS 4 microspheres CE demonstrated the lowest charge transfer resistance and highest electrocatalytic activity for the I 3 − /I − redox couple reaction. The NiMoS 4 -based DSSC showed a higher power conversion efficiency (8.9%) even than that of Pt-based DSSC (8.7%) under simulated standard global AM 1.5 G sunlight (100 mW cm − 2 ). As an electroactive material for SCs, the assembled NiMoS 4 //AC asymmetric supercapacitor showed excellent specific capacitance (118.7 F g − 1 at 1 A g − 1 ) , high energy density of 42.2 Wh kg − 1 (with a power density of 799.2 W kg − 1 ) , and superior cycling durability with a specific capacitance retention of 79.5% after 9000 cycles at 3 A g − 1 .
研究领域:
材料科学
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能源技术
·
电化学
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Huiru Yang,Linyuan Zhou,Honggang Chen,Yan Zeng,Dan Li,Changwei Hu
Primary amines are vital building blocks in pharmaceutical and polymer industry. The heterogeneous catalytic hydrogenation of aliphatic acyclic amides to amines is rather attractive but challenging due to low reactivity of aliphatic acyclic amides, and then rarely be reported. Herein, cheap bimetallic NiMo nitride catalysts were synthesized by hydrothermal method and firstly utilized to the efficient conversion of a wide range of aliphatic acyclic amides to amines, achieving 93.9 % conversion of hexanamide and 75.1 % yield to hexylamine. Characterizations such XRD, N 2 Physical adsorption, TGA, Raman, XPS, SEM-EDX Mapping and (HR)TEM revealed that Ni 2 Mo 3 N is crucially important for the activation of hexanamide while the synergetic effect between Ni 2 Mo 3 N and Ni 6 Mo 6 C 1.06 would further promote the conversion of hexanamide, and higher TOFs (145.9 h −1 ) and lower Ea (29.5 kJ mol −1 ) are achieved. The C O bond of the amide can be activated by the surface Lewis acid site of bimetallic NiMo nitrides , while the simultaneous dissociation of H 2 to form H atoms is beneficial for hydrogenation. This catalyst is also found to be recyclable with stable catalytic performance upon consecutive runs. The present work provides a novel and unique option for the efficient conversion of aliphatic acyclic amides to amines, being a strong supplementary to those reported for the hydrogenation of cyclic-amides, secondary amides, and tertiary amides.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xueqin Gong,Fengxia Tong,Fahao Ma,Yujia Zhang,Peng Zhou,Zeyan Wang,Yuanyuan Liu,Peng Wang,Hefeng Cheng,Ying Dai,Zhaoke Zheng,Baibiao Huang
Photoreforming of plastic waste is a novel approach, which can not only degrade plastic waste into valuable chemicals, but also produce high-energy-density hydrogen fuels. Here, we developed an in-situ derived carbon nitride-carbon nanotubes-NiMo hybrids via NiMo-assisted catalysis route, which works as an efficient and stable photocatalyst for plastics photoreforming. The strong π-π interaction between in-situ derived CNTs and CN promotes electron transfer, increases carrier lifetime and improves photocatalytic activity. The DFT calculations and single-particle PL quenching phenomenon confirmed the strong interface effect and charge transport for CN-CNTs-NM. In addition, the strong interaction between photocatalyst and ethylene glycol in plastics was observed in situ by single-particle PL. This work provides a smart strategy of utilizing in-situ derived π-π interaction as well as direct evidence of the charge transfer from the photocatalysts to ethylene glycol , which provides guidance for the rational design of highly efficient photocatalysts for plastics photoreforming.
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Materials
·
2023
·Vol. 16
·期 8
·3171
·
IF 3.4
Hongbin Wang,Beirong Ye,Chen Li,Tao Tang,Sipu Li,Shaojun Shi,Chunyang Wu,Yongqi Zhang
Water electrolysis as an important and facile strategy to generate hydrogen has attracted great attention, and efficient electrocatalysts play a key role in hydrogen evolution reaction (HER). Herein, vertical graphene (VG)-supported ultrafine NiMo alloy nanoparticles (NiMo@VG@CC) were fabricated successfully via electro-depositing as efficient self-supported electrocatalysts for HER. The introduction of metal Mo optimized the catalytic activity of transition metal Ni. In addition, VG arrays as the three-dimensional (3D) conductive scaffold not only ensured high electron conductivity and robust structural stability, but also endowed the self-supported electrode large specific surface area and exposed more active sites. With the synergistic effect between NiMo alloys and VG, the optimized NiMo@VG@CC electrode exhibited a low overpotential of 70.95 mV at 10 mA cm−2and a remarkable stable performance over 24 h. This research is anticipated to offer a powerful strategy for the fabrication of high-performance hydrogen evolution catalysts.Keywords:vertical graphene;NiMo alloy;high surface area;hydrogen evolution reaction;electrodeposition
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