ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Longfei Zhu,Sen Ye,Jiazheng Zhu,Chengjie Duan,Kun Li,Guangke He,Xiang Liu
Developing highly active nonnoble-metal-based heterogeneous catalysts for selective hydrogenation is a long-sought goal due to the scarcity and high price of noble metals. Herein, well-dispersed and small-sized Ni nanoparticles (NPs) supported on hydroxyapatite (Ni-TA/HAP) were prepared using a simple tartaric acid (TA)-assisted impregnation method, which is based on the coupling interaction of strong electrostatic adsorption between the HAP and TA and reactive metal–ligand chelation between Ni and TA. Under mild conditions (e.g., 1 mol % Ni, 3 bar H2 at 80 °C), the as-synthesized Ni-TA/HAP exhibited excellent activity and selectivity (>99%) for the efficient hydrogenation of phenolic compounds to the corresponding cyclohexanols, as well as the controlled partial hydrogenation of N-heteroarenes. Characterization results revealed that TA addition could promote a better dispersion of Ni species and inhibit the aggregation of Ni NPs during the fabrication of the Ni-TA/HAP catalyst. An optimal TA dosage (nTA/nNi = 0.5) as well as a low Ni loading (1.0 wt %) coconstructed the favorable microstructure of the well-dispersed Ni nanoparticles as the catalytic center. The hydrogenation was boosted by small-sized Ni nanoparticles with a high ability for H2 activation and HAP with both base and acid sites for appreciating phenol absorption.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 24
·7943-7954
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IF 6.119
Hao Zhang,Xiaojing Song,Hao Sun,Zhenyu Lei,Shouxin Bao,Chen Zhao,Dianwen Hu,Wenxiang Zhang,Jingyao Liu,Mingjun Jia
Developing highly efficient and durable eco-friendly heterogeneous catalysts for the Friedel–Crafts acylation (FCA) reaction has been a long-term and significant target, yet remains a great challenge. Herein, a series of Fe–Ni alloy nanoparticles (NPs) encapsulated inside N-doped carbon spheres (FexNi1−x@NC) was rationally fabricated by pyrolyzing the Fe–Ni bimetallic metal–organic frameworks (BMOFs-FexNi1−x) to this end. Various characterization results demonstrated that FeNi alloy NPs (25 nm) covered by a thin carbon shell (5 nm) were uniformly distributed throughout the entire carbon-based composite. A number of oxidized metal species (Fe3+, Ni2+) are present on the surface of the inner bimetallic core, which should be the main source of catalytically active centers of the carbon-wrapped metal NP catalysts. The composition-optimized Fe0.8Ni0.2@NC with relatively higher positive surface charges exhibited the highest catalytic activity and excellent stability for the acylation of aromatic compounds with acyl chlorides. The density functional theory calculations revealed that the catalytic activity of the FexNi1−x@NC catalysts could arise from the electron transfer, i.e., from the outermost layer of the carbon shell to the inner positively charged Fe-based metal NPs, which can lead to a positive charge distribution (by acting as weak Lewis acid sites) on the external surface of the carbon-encapsulated metal NP catalysts. In this case, the external carbon shell can function as ‘chainmail’ to transfer the Lewis acidity (positive charge), and also to protect the inner metal core from the destructive reaction environment, thus resulting in the formation of highly efficient and durable FCA catalysts.
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CHEMBIOCHEM
·
2021
·Vol. 23
·期 4
·e202100497
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IF 3.164
Kangjing Wang,Liting Zhao,Ting Li,Qian Wang,Zhongyang Ding,Weifu Dong
Graphical Phosphomannose isomerase (PMI) with His-tag was successfully immobilized on Ni 2+ charged pyridine-derived particles. The immobilized enzymes effectively maintained their activity. Excellent reusability and stability was observed after immobilization. Self-stable precipitation polymerization was used to prepare an enzyme-immobilized microsphere composite. Phosphomannose isomerase (PMI) with His-tag was successfully immobilized on Ni 2+ charged pyridine-derived particles. The maximum amount of PMI immobilized on such particles was ∼184 mg/g. Compared with free enzyme, the activity of the immobilized enzymes was significantly improved. In addition, the immobilized enzymes showed a much better thermostability than free enzymes. At the same time, the immobilized enzymes can be reused for multiple reaction cycles. We observed that the enzyme activity did not decrease significantly after six cycles. We conclude that the pyridine-derived particles can be used to selectively immobilize His-tagged enzymes, which can couple the enzyme purification and catalysis steps and improve the efficiency of enzyme-catalyzed industrial processes.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Xiaolan Li,Yang Liu,Jinliang Zhu,Panagiotis Tsiakaras,Pei Kang Shen
Herein, we introduce a facile approach to synthesize a unique class of Pt-M (M = Ni, Co) catalysts with a nanoflower structure for boosting both oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR). By controlling the surface-active agents, we modified the functional groups surrounding the Pt atoms, tuned the alloying of Pt and the transition metals Ni and Co, and prepared two different kinds of nanodendrites. Their successful synthesis depends on the selection and amount of surfactants (hexadecyltrimethylammonium bromide (CTAB), Polyvinylpyrrolidone (PVP)). Besides, by controlling reaction time, we also explored the forming procedures for Pt-Co globularia nanodendrite (Pt-Co GND) and Pt-Ni petalody nanodendrite (Pt-Ni PND). Our investigation highlights the importance of complex nanoarchitecture, which enables surface and interface modification to achieve excellent catalytic performance in fuel cell electrocatalysis. The characterization of the as-prepared catalysts reveals a high electrochemical surface area and mass activity (2041 m A m g P t - 1 and 950 m A m g P t - 1 for Pt-Co GND and Pt-Ni PND, respectively, for ORR). Furthermore, Pt-Co GND showed a high MOR activity, with a mass activity value recorded at 1615 m A m g P t - 1 which is far superior to that for Pt/C. Moreover, both catalysts retain high activity after accelerated durability tests (ADTs). The electron transfer number was calculated by performing the rotating ring-disk electrode (RRDE) measurements. Due to abundant active sites of Pt, both Pt-Co GND and Pt-Ni PND exhibit a 4e − pathway for ORR with electron transfer number of >3.95.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Jiang Liao,Ao Ju,Wenhao Jiang,Yan Ju,Xueliang Liu,Nianxiang Hu,Ruidong Xu,Junli Wang
Transition metal hydroxides, due to their low cost and high theoretical capacity, are promising candidates for supercapacitors . However, the lower conductivity of hydroxides usually results in devices exhibiting poor specific capacity. Here, Ni(OH) 2 @Ni 12 P 5 electrodes are designed and prepared, showing great potential for applications. This composite electrode, prepared by simple phosphating treatment and electrodeposition . Compared with the Ni(OH) 2 prepared by direct deposition, this rationally designed electrode exhibits more excellent electrochemical properties. The prepared Ni(OH) 2 @Ni 12 P 5 electrode exhibits a good area specific capacitance of 15.89 F•cm −2 at a current density of 10 mA•cm −2 , which is 2.93 times higher than that of the Ni(OH) 2 electrode (5.43 F•cm −2 ). In addition, the assembled Ni(OH) 2 @Ni 12 P 5 //AC asymmetric supercapacitor exhibits an energy density of 0.38 mWh•cm −2 at a power density of 8.00 mW•cm −2 . Therefore, this work provides a new strategy for the synthesis of high-performance supercapacitor electrodes.
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Scientific Reports
·
2021
·Vol. 11
·期 1
·1-11
·
IF 4.38
Wang Haitao,Zou Haiyan,Liu Yingying,Liu Zhenglong,Sun Wenshuang,Lin Kunyi Andrew,Li Tielong,Luo Shuangjiang
It’s highly desired but challenging to synthesize self-supporting nanohybrid made of conductive nanoparticles with metal organic framework (MOF) materials for the application in the electrochemical field. In this work, we report the preparation of Ni 2 P embedded Ni-MOF nanosheets supported on nickel foam through partial phosphidation (Ni 2 P@Ni-MOF/NF). The self-supporting Ni 2 P@Ni-MOF/NF was directly tested as electrode for urea electrolysis. When served as anode for urea oxidation reaction (UOR), it only demands 1.41 V (vs RHE) to deliver a current of 100 mA cm −2 . And the overpotential of Ni 2 P@Ni-MOF/NF to reach 10 mA cm −2 for hydrogen evolution reaction HER was only 66 mV, remarkably lower than Ni 2 P/NF (133 mV). The exceptional electrochemical performance was attributed to the unique structure of Ni 2 P@Ni-MOF and the well exposed surface of Ni 2 P. Furthermore, the Ni 2 P@Ni-MOF/NF demonstrated outstanding longevity for both HER and UOR. The electrolyzer constructed with Ni 2 P@Ni-MOF/NF as bifunctional electrode can attain a current density of 100 mA cm −2 at a cell voltage as low as 1.65 V. Our work provides new insights for prepare MOF based nanohydrid for electrochemical application.
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MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING
·
2021
·
IF 5.234
Xiaoyu Zhang,Ying Liu,Xiaobo Liu,Jingfan Zhang,Xin Chen,Yanxia Wu,Lin Jing,Xiaolei Wu,Min Zhao,Peide Han
Few-layer graphene reinforced nickel matrix (GNs/Ni) composites were fabricated by a facile in-situ processing strategy involving the transformation from solid carbon precursors to graphene reinforcements under the vacuum hot-press sintering. It enabled the homogeneous distribution of reinforcements, the effective interfacial bonding between graphene nanosheets and Ni matrix, as well as the resisted grain growth during the high-temperature consolidation process. The GNs/Ni composites exhibited exceptionally enhancement of the strength and ductility simultaneously. The composite with 0.3 wt% graphene achieved the optimal yield strength, tensile strength , and fracture elongation of 285 MPa, 611 MPa, and 56%, respectively, which were enhanced by 1.16, 1.34 and 1.37 folds compared to those of pure Ni bulk. The microstructures before and after tensile deformation demonstrated that the strengthening effect of in-situ grown graphene in the Ni matrix was attributed to the grain refinement and effective load transfer, while the toughening effect was related to the crack bridging and graphene pull-out mechanisms.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Zonglin Liu,Baoqiang Li,Yujie Feng,Dechang Jia,Caicai Li,Qingfeng Sun,Yu Zhou
Reasonable design and facile synthesis of high-efficiency non-noble electrocatalysts for hydrogen evolution reaction (HER) in water splitting are crucial for renewable and clean energy technologies. Increasing the number of active sites via nanostructuring is a fundamental method to promote the HER activity of the catalysts. However, the balance between the exposed active sites and the stability cannot be well maintained due to the aggregation of nanoscale catalysts. Therefore, it is imperative to combine effective active compounds with suitable carbon materials to stabilize nanomaterials. Hence, a hybrid architecture with Ni(PO 3 ) 2 nanoparticles ladened on the carbon nanotubes (Ni(PO 3 ) 2 /CNTs) was elaborately designed and synthesized by pyrolyzing the nickel phthalocyanine (NiPc)/CNTs assemblies and subsequent phosphidation. The π-π interaction between NiPc and CNTs is conductive to the tight attachment of the active species to the substrate, while the inlaid structure effectively prevents the corrosion/aggregation of Ni(PO 3 ) 2 nanoparticles and ensures the stability of the catalyst. Accordingly, Ni(PO 3 ) 2 /CNTs displayed excellent HER performances with remarkable stability both in 1.0 M KOH and 0.5 M H 2 SO 4 with overpotentials of 71 mV and 87 mV at 10 mA cm −2 , respectively. The Tafel slopes of Ni(PO 3 ) 2 /CNTs in alkaline and acid medium were 65 mV dec -1 and 46 mV dec -1 , respectively, both exposed a Volmer-Heyrovsky mechanism during the HER. The present work will shed new light on the exploitation of non-noble metal high-efficiency HER electrocatalysts.
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E-POLYMERS
·
2021
·Vol. 21
·期 1
·590-605
·
IF 2.025
Li Zhao,Xianzhi Hu,Futing Zi,Yingmei Liu,Deqiong Hu,Peng Li,Huiling Cheng
In this study, a novel functional monomer N -(1-(2,4-difluorophenyl)-2-(1 H -1,2,4-triazol-1-yl)ethyl)acrylamide (NDTEA) was designed and synthesized, and was used to prepare Ni( ii ) ion-imprinted polymers (Ni( ii )-IIPs). Sixteen kinds of Ni( ii )-IIP (Ni( ii )-IIP 1–16 ) and corresponding non-imprinted polymers (NIP 1–16 ) were prepared by precipitation polymerization method. After optimized condition experiment, Ni( ii )-IIP 5 possessed maximum adsorption capacity and better imprinting factor under optimal experimental conditions which indicated by equilibrium adsorption experiments. The morphology and structural characteristics of Ni( ii )-IIP 5 were characterized by scanning electron microscopy (SEM) and Brunauer–Emmett–Teller (BET). The adsorption selectivity of Ni( ii )-IIP 5 was analyzed by ICP-OES, and the results showed that Ni( ii )-IIP 5 had favorable selectivity recognition ability for Ni( ii ) when Cu( ii ), Co( ii ), and Cd( ii ) are used as competitive ions. The kinetic experiment indicated that the performance of Ni( ii ) adsorption on the surface of Ni( ii )-IIP 5 obeyed the pseudo-first-order model, and adsorption equilibrium was attained after 15 min. Isothermal adsorption process fitted to Langmuir and Freundlich isothermal adsorption models, simultaneously. The results showed that Ni( ii )-IIP 5 prepared by using a new functional monomer had better permeation selectivity and higher affinity for Ni( ii ), which also verified the rationality of the functional monomer design. At the same time, it also provided a broad application prospect for removal of Ni( ii ) in complex samples.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yongxin Qian,Yang Tao,Wang Li,You Li,Tian Xu,Jinian Hao,Qinghui Jiang,Yubo Luo,Junyou Yang
Electronic packaging materials with efficient heat dissipation and anti-electromagnetic-interference performance are highly desirable to realize the long-term stable operation of highly integrated electronic devices. Such combined functions of heat dissipation and anti-electromagnetic-interference are achieved here by filling 3D CNF@C-Ni network skeleton in epoxy resins (EP). The CNF@C-Ni is a carbon nanofibers network skeleton embedded with micron flower-like C-Ni particles and has been obtained by carbonizing nickel metal–organic frameworks (Ni-MOF) embellished bacterial cellulose. The 3D CNF@C-Ni network skeleton provides a highly efficient heat transfer channel for EP, rendering a high thermal conductivity of 0.5 W·m −1 K −1 at room temperature for the 5 wt% CNF@C-Ni filled EP, ~2.8 times higher than that of pristine EP. In addition, the flower-like C-Ni particles realize an optimization in the impedance matching of CNF@C-Ni/EP, enabling a high electromagnetic wave absorption performance in the wave-transparent epoxy resins. In particular, a lowest reflection loss value of −49.77 dB at 13.44 GHz with a maximum effective bandwidth of 5.44 GHz (from 12.08 to 17.52 GHz) has been achieved in the 5 wt% CNF@C-Ni filled epoxy resins with a thickness of 2.2 mm. Such a new dual-functionated epoxy resin with combined high electromagnetic wave absorption and thermal management performance shows great potential in manufacturing of highly integrated electronic devices.
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FUEL
·
2021
·
IF 6.609
Zier Jin,Hong Xia,Wenxin Yang,Mingen Liu,Xiaoyu Liu,Jiao Xiang,Abdul Qayum,Liangsheng Hu,Lianfeng Duan,Wenhua Gao,Zhi Liu,Fushen Lu
Ammonia borane (NH 3 BH 3 , AB) has been considered as one of the most attractive candidates for chemical hydrogen-storage materials. Development of low-cost and high-performance catalysts for hydrogen generation from AB is highly desirable, which is still a huge challenge. Herein, Ru-Ni bimetallic nanoparticles were fabricated on (3-aminopropyl) triethoxysilane-functionalized reduced graphene oxide nanosheet (APTS-rGO) by a facile one-step in situ co-reduction strategy. The newly developed Ru 1 Ni 4 /APTS-rGO catalyst with hydrophilic interface and narrow particle size-distribution presented a remarkably enhanced catalytic activity for hydrolytic H 2 generation from AB, affording an ultra-high TOF value of 1559 min −1 . The APTS-rGO support was effective to minimize the aggregation of Ru-Ni nanoparticles, achieving the immobilization of ultrasmall Ru-Ni nanoparticles (2.0 nm) on support surface. The change in local charge density of catalyst surface caused by Ru-Ni synergistic effect and metals-support interaction improved the catalytic performance of Ru 1 Ni 4 /APTS-rGO. Hydrophilic NH 2 -containing interface ensured high dispersibility of catalysts in reaction solution, increasing the contact opportunities between active sites and AB molecules. These factors contributed together to the exceptional catalytic performance of Ru 1 Ni 4 /APTS-rGO. This catalytic system has potential applications in various catalytic fields due to its obvious advantages of the facile preparation method, good hydrophilicity, and the outstanding catalytic performance.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2021
·
IF 5.541
Haimiao Yu,Jiecheng Liu,Haojie Yang
A novel magnesium slag (MS) supported nickel-based catalysts (Ni/MS) was prepared and tested in catalytic reforming of volatiles derived from the pyrolysis of biomass components (cellulose, hemicellulose and lignin) and two biomass feedstocks (pine and straw). The physical and chemical properties of catalysts were characterized by XRD, TPR, BET, TEM, TPO-TGA and Raman spectroscopy. Ni/MS catalyst showed a higher tar removal efficiency than conventional Ni/γ-Al 2 O 3 under the same Ni loading. The tar conversion of cellulose hemicellulose and lignin reached 94.8 %, 92.0 % and 89.4 %, respectively over Ni/MS catalyst. In addition, the lignin content of the biomass feedstock appreciably affected the yield and dew point of tar. The highest increment in gas and H 2 yield (increased by 39.0 % and 106.4 %, respectively) was observed in cellulose. The highest decrement in tar dew point (from 166.4 ℃ to 53.0 ℃) was observed in hemicellulose. The excellent tar removal of Ni/MS was attributed to the metallic Ni and Ni-Fe alloy on catalyst surface. Besides, the MgO and Fe 2 O 3 phases in the support can retard the carbon deposition during the reaction. The results of this study are expected to provide insightful guidance for the application of Ni/MS catalysts for pyrolysis/gasification of biomass.
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