APPLIED SURFACE SCIENCE
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2025
·
IF 6.9
Pingping Wu,Lei Song,Xingwang Zhang,Yingqi Zhang,Peng Bai,Lianming Zhao,Zifeng Yan
The balance between catalytic activity and product selectivity remains a challenge in partial oxidation reactions, because its products are prone to be further oxidized. In this paper, a small amount of Ni was introduced on the surface of the supported AuPd alloy nanoparticles (NPs) as a promoter to construct the Ni/AuPd interface for benzyl alcohol partial oxidation, which helped to improve the selectivity of benzaldehyde. The results showed that the introduction of a small amount of Ni (<0.5 wt%) led to no obvious change of the catalytic activity, but the selectivity of benzaldehyde was greatly improved. When Ni content exceeds 1.0 wt%, the benzyl alcohol conversion decreased significantly. This is mainly because a large amount of Ni led to an obvious aggregation of Pd on the catalyst and a large amount of surface Ni species partially covered the active components, resulting in a low catalytic activity. Introducing a small amount of Ni improved the benzaldehyde selectivity and Ni species presented as NiO and NiOOH on catalyst xNi/AuPd/MCF-H. Theoretical calculation results show that the improved benzaldehyde selectivity was attributed to the easy desorption of benzaldehyde from NiO and NiOOH surfaces.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Haitao Wang,Hong Zhu,Zhenggang Bu,Kai Dan,Chaofeng Shen,Liping Lou
Co-doping with non-metallic and metallic elements offers an effective strategy to address the inherent limitations of zero-valent iron (ZVI) materials, including low reactivity and selectivity towards target contaminants and surface passivation. This study synthesized high-performance sulfur-nickel co-doped microscale ZVI (S-Ni-mZVI) through a facile and cost-effective one-step ball milling method to achieve high dehalogenation activity. A comprehensive comparative analysis between mZVI, S-mZVI, and Ni-mZVI revealed the superior trichloroethylene (TCE) degradation kinetics, electron efficiency, pH tolerance, and long-term activity of S-Ni-mZVI. Specifically, S-Ni-mZVI achieved a pseudo-first-order TCE degradation rate constant of 1.05 h −1 (>97 % removal in 4 h), outperforming mZVI by 150.9-fold, and exhibited an electron efficiency of 70.7 %. Mechanistically, S (FeS) effectively suppressed hydrogen evolution (up to 99.3 % inhibition) and passivated Ni-induced hydrogenolysis, and Ni (Ni-Fe galvanic couple) augmented the electron cloud density of sulfur and synergistically promoted electron transfer in conjunction with FeS, resulting in a 6.4-fold rate acceleration. Furthermore, the co-doping of S and Ni induced Fe⁰ lattice contraction, significantly enhancing the material’s corrosion resistance. Additionally, S-Ni-mZVI exhibited broadened pH adaptability and sustained long-term degradation performance, maintaining a TCE removal rate exceeding 98 % over 13 days. Moreover, the leaching concentration of Ni remained consistently below 0.2 mg·L −1 , confirming the environmental friendliness of the material. Electrochemical analysis and kinetic isotope effect studies further revealed that Ni-mZVI degraded TCE primarily via hydrogenolysis. In contrast, S-mZVI and S-Ni-mZVI mainly employed direct electron transfer ( β -elimination). This work offers a pragmatic and scalable strategy for engineering highly active, electron-efficient, and durable ZVI-based materials for efficient remediation of chlorinated hydrocarbons.
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CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Caihong Wang,Weiliang Qi,Ying Zhou,Wandi Kuang,Tamil Azhagan,Tiju Thomas,Chunjie Jiang,Siqi Liu,Minghui Yang
Efficient semiconductor-cocatalyst junctions are of direct relevance to solar energy based fuel generation. Here, Ni-Mo ternary nitrides based one-dimensional hierarchical structures (In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni)) have been successfully prepared and used to achieve visible light driven H 2 evolution. Because of the metallic-like properties of the transition metal nitrides, Ni 0.2 Mo 0.8 N(Ni) as co-catalysts can promote photo-generated charge-carriers transportation/separation and decrease the overpotential of H 2 -evolution. Thus, the photocatalytic property of optimal 1 wt% In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni) exhibits a hydrogen evolution rate of 614.2 μmol g -1 h −1 , which is about 10 times as high as that of blank In 2 S 3 (61.4 μmol g −1 h −1 ). Besides, the pure Ni 0.2 Mo 0.8 N shows higher co-catalytic properties than Ni 0.2 Mo 0.8 N(Ni). This indicates that the metallic Ni (and related species) lowers the co-catalytic role of ternary nitrides. Another robust indication of this is the fact that In 2 S 3 -Ni 0.2 Mo 0.8 N nanohybrid displays about 2 times higher H 2 evolution rate than In 2 S 3 -Ni 0.2 Mo 0.8 N(Ni).
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ELECTROCHIMICA ACTA
·
2022
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IF 7.336
Yuqi Yan,Qinghai Ma,Fang Cui,Jiajia Zhang,Tieyu Cui
High-performance carbon onions coated Ni/NiO nanoparticles (CNN NPs) acting as electrocatalysts in alkaline hydrogen evolution reaction (HER) is synthesized base on a self-assembly process combined with a calcination process. By systematically regulating the surface composition, we find that controlling the kinetic steps in HER by regulating the ratio of Ni/NiO can significantly promote alkaline HER activity, and CNN-500 with a Ni/NiO ratio of 1.31 display an overpotential of 127 mV (vs. RHE) at a current density of 10 mA cm −2 for HER in 1 M KOH electrolyte. The ratio of Ni and NiO active catalytic components are adjustable via controlling the calcination process, which play an important role in alkaline HER performance. Due to the synergistic effect between Ni, NiO and C, the CNN-500 shows superior intrinsic catalytic activity than that of currently reported HER electrocatalysts. This work provides a facile and useful strategy to get high-performance alkaline HER electrocatalysts for hydrogen energy source.
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International Journal of Minerals Metallurgy and Materials
·
2022
·Vol. 30
·期 1
·54-62
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IF 3.85
Xu Nuo,Yuan Zirui,Ma Zhihong,Guo Xinli,Zhu Yunfeng,Zou Yongjin,Zhang Yao
MgH 2 with a large hydrogen capacity is regarded as a promising hydrogen storage material. However, it still suffers from high thermal stability and sluggish kinetics. In this paper, highly dispersed nano-Ni has been successfully prepared by using the polyol reduction method with an average size of 2.14 nm, which significantly improves the de/rehydrogenation properties of MgH 2 . The MgH 2 —10wt% nano-Ni sample starts releasing H 2 at 497 K, and roughly 6.2wt% H 2 has been liberated at 583 K. The rehydrogenation kinetics of the sample are also greatly improved, and the adsorption capacity reaches 5.3wt% H 2 in 1000 s at 482 K and under 3 MPa hydrogen pressure. Moreover, the activation energies of de/rehydrogenation of the MgH 2 —10wt% nano-Ni sample are reduced to (88 ± 2) and (87 ± 1) kJ·mol −1 , respectively. In addition, the thermal stability of the MgH 2 —10wt% nano-Ni system is reduced by 5.5 kJ per mol H 2 from that of pristine MgH 2 . This finding indicates that nano-Ni significantly improves both the thermodynamic and kinetic performances of the de/rehydrogenation of MgH 2 , serving as a bi-functional additive of both reagent and catalyst.
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JOURNAL OF SOLID STATE CHEMISTRY
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2023
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IF 3.3
Yuwei Chen,Jingcheng Feng,Feidi Fan,Jun Shen,Guochun Zhang,Heng Tu
Three new transition-metal-based borate crystals, Li 5 MgSrMB 12 O 24 (M = Cr, Ni) and Li 5 ZnSrNiB 12 O 24 , were obtained using the high temperature solution method. Their structures were determined by the single crystal X-ray diffraction, which crystallize in the trigonal R 3 ¯ space group. The [B 3 O 11 ] groups in the structures lead to the long distance between two nearest magnetic ions, which can reduce the interaction of adjacent magnetic centers. The magnetic properties and thermal stabilities of the title compounds were also investigated. The results indicated that Li 5 MgSrCrB 12 O 24 has stable chemical-physical properties and its maximum –ΔS m value of 14.33 J kg −1 ·K −1 at 2 K for Δμ 0 H = 9 T reaching 88.6% of the theoretical paramagnetic limit, suggesting its potential application on the magnetic refrigeration.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Lu Zhang,Guijiu Xie,Fuyi Liu,Huiming Ji
Hydrogen sensors are very important for real-time detection of hydrogen leakage. In this study, a Pd-Ni film hydrogen sensor with high hydrogen response and selectivity was fabricated. A 1.3 µm-thick organosilica membrane was coated on the surface of Pd-Ni alloy film by sol-gel process and hot-coating method to fabricate a 1,2-bis(triethoxysilyl)methane (BTESM)-coated Pd-Ni film hydrogen sensor, which endows the sensor with superior H 2 selectivity due to the molecular sieve property. And the gas sensing performance was tested at optimum operating temperature. The results show higher response is obtained in both N 2 and air atmosphere by hybrid organosilica membrane modification on the Pd-Ni film sensor. Very importantly, the response of the sensor to hydrogen is greatly improved and well maintained in the presence of oxygen, although the response/recovery time increased. The organosilica membrane has high permeability to hydrogen with the kinetic dimater of 0.289 nm while effectively inhibits the permeation of relatively larger gas molecule such as oxygen (0.34 nm) and methanol (0.38 nm), resulting in excellent selectivity to H 2 . The mechanism of response and selectivity enhancement is explored.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Jianhua Yu,Xiancai Pang,Qunchao Yin,Di Chen,Hongzhou Dong,Qian Zhang,Jing Sui,Lina Sui,Lifeng Dong
Constructing self-supporting porous electrode material with abundant electrochemical active sites can effectively improve the energy storage capacity of supercapacitors . Herein, a novel electrode material (NCS@Co-ZIF/NF) is developed by depositing zeolitic imidazolate frameworks (Co-ZIF) on nickel foams (NF), which is adopted as a precursor (Co-ZIF/NF) to electrodeposit nickel-cobalt sulfides (NCS). The nanosheet arrays with cross-porous structures provide NCS@Co-ZIF/NF with excellent electrochemical characteristics, including a high specific capacity of 144.4 mAh g −1 at the current density of 1 mA cm −2 , 60.5% capacity retention at 50 mA cm −2 , and superb long-term cycle stability. Furthermore, NCS@Co-ZIF/NF//AC hybrid supercapacitor is fabricated by using NCS@Co-ZIF/NF as positive electrodes and activated carbon (AC) as negative electrodes , which exhibits a high energy density of 33.9 Wh kg −1 at a power density of 145 W kg −1 .
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2021
·Vol. 45
·期 10
·14985-14994
·
IF 5.164
Siqi Qiu,Renbo Guo,Qingyu Wang,Feng Yang,Yibo Han,Xiaoniu Peng,Hui Yuan,Xina Wang
Summary P-type Ni(OH) 2 has been combined with n-type CdS nanorods and nanocrystals for enhanced photocatalytic property due to the p-n junction. Though CdS nanosheets exhibit fast charge transfer and large superficial area, the decoration of Ni(OH) 2 was rarely reported up to now. In this work, the photo-deposition of Ni(OH) 2 nanoparticles on CdS ultrathin nanoflakes was established for efficient photocatalytic H 2 generation. By changing the irradiation time of CdS, the reaction between Ni 2+ and OH − can be controlled for different loading density of Ni(OH) 2 . As the loading density-dependent morphology, light absorption, carrier separation and transfer were systematically studied for the composites, an obvious band gap narrowing from 2.28 to 2.08 eV was revealed, and the carrier separation and transfer between the CdS nanoflakes and Ni(OH) 2 nanoparticles have been enhanced for the composites with deposition time of 3 minutes. These together with the alignment of type “II” bands and the high specific surface area of the flakes and nanoparticles, lead to an optimum H 2 generation of 20.14 mmol/g/h, nearly three times of pure CdS (7.97 mmol/g/h). Such a study not only provides a deposition method of Ni(OH) 2 , but also sheds light on the enhancement strategy for photocatalytic property by controlling the microstructure and aligning the hetero-structured bands.
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JOURNAL OF POWER SOURCES
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2022
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IF 9.794
Yao Lv,Shifei Huang,Sirong Lu,Wenbo Ding,Xiaoliang Yu,Gemeng Liang,Jinshuo Zou,Feiyu Kang,Jiujun Zhang,Yidan Cao
Ni-rich layered oxide material with high theoretical capacity and low cost is one of the most promising cathode candidates for high-energy-density lithium-ion battery. However, increase of Ni content triggers structural instability and fast capacity degradation, which severely impedes the practical application of Ni-rich materials. Here, a surface dual-modification layer of B 2 O 3 & LiBO 2 is introduced to Ni-rich material LiNi 0.89 Co 0.08 Mn 0.03 O 2 (NCM89), which successfully stabilizes the layered structure of NCM89 during cycling as well as removes residual lithium in NCM89. The in-situ X-ray diffraction and cross-sectional scanning electron microscopy results demonstrate effectively improved structural reversibility and stability of the cathode. Moreover, the dissolution of transition metals and decomposition of electrolyte at the cathode/electrolyte interface are successfully suppressed, resulting in beneficial cathode electrolyte interphase (CEI) layer. As a result, the boron modified cathode exhibits s a high capacity of 180.4mAh g −1 along with an excellent capacity retention of 90% after 100 cycles at 1C in 2.75–4.35 V at 25 °C, while the pristine NCM89 cathode only retains 59% of its initial capacity after 100 cycles. Furthermore, the capacity retention of full cell after 350 cycles is improved from 52.5% to 90%.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 22
·15547-15554
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IF 3.3
Changyin Zhong,Yifei Yang,Yun Fang,Jun Chen,Bomin Feng,Hongbing Wang,Wenhua Luo,Yunxi Yao
Lanthanum oxide (La2O3) possesses superior reactivity during catalytic hydrogenation, but the intrinsic activity of La2O3 toward H2 adsorption and activation remains unclear. In the present work, we fundamentally investigated hydrogen interaction with Ni-modified La2O3. Hydrogen temperature programmed desorption (H2-TPD) on Ni/La2O3 shows enhanced hydrogen adsorption with a new hydrogen desorption peak at a higher temperature position compared to that on the metallic Ni surfaces. By systematically exploring the desorption experiments, the enhanced H2 adsorption on Ni/La2O3 is due to the oxygen vacancies formed at the metal–oxide interfaces. Hydrogen atoms transfer from Ni surfaces to the oxygen vacancies to form lanthanum oxyhydride species (H–La–O) at the metal–oxide interfaces. The adsorbed hydrogen at the metal–oxide interfaces of Ni/La2O3 results in improved catalytic reactivity in CO2 methanation. Furthermore, the enhanced hydrogen adsorption on the interfacial oxygen vacancies is ubiquitous for La2O3-supported Fe, Co, and Ni nanoparticles. Benefiting from the modification effect of the supported transition metal nanoparticles, the surface oxyhydride species can be formed on La2O3 surfaces, which resembles the recently reported oxyhydride observed on the reducible CeO2 surfaces with abundant surface oxygen vacancies. These findings strengthen our understanding of the surface chemistry of La2O3 and shed new light on the design of highly efficient La2O3-based catalysts with metal–oxide interfaces.
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CATALYSIS TODAY
·
2022
·
IF 6.562
Zhuangqing Wang,Xinchao Wang,Chao Zhang,Yinze Yang,Leilei Zhou,Haiyang Cheng,Fengyu Zhao
Catalytic conversion of furfural and its derivatives to value-added C 5 molecules has attractive much attention in the field of biomass conversion . In this paper, the selective hydrogenolysis of tetrahydrofurfuryl alcohol to 1,5-pentanediol has been studied over a series of PrO x promoted Ni/Al 2 O 3 catalysts. The catalytic performances and the promoting effects of PrO x , as well as the role of Ni and PrO x species have been discussed. The surface properties and structure of catalysts were examined by TEM, XRD, XPS, H 2 -TPR, H 2 -TPD, in-situ DRIFTS, etc. The presence of PrO x species promotes the reaction rate and changes product selectivity significantly, and a 79.2% 1,5-pentanediol selectivity can be obtained at 88.4% conversion over the NiPr 1.2 /Al 2 O 3 catalyst. The synergistic effect between defect-rich PrO x and the adjacent active Ni species has been confirmed to contribute to the superior catalytic performances. These results provide useful knowledge for the activation of cyclic ether bonds and the design of heterogeneous catalysts with lanthanide oxide supports.
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