SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yi Wang,Qingjie Ji,Jixiang Xu,Jun Wan,Lei Wang
In this study, N-doped porous carbon materials embedded with NiN x species (Ni@NC) were fabricated via the pyrolysis of Ni-doped zeolitic imidazolate frameworks-8 (ZIF-8) at the temperature of 900 °C. The obtained Ni@NC-1 catalyst exhibited excellent activity in activating the peroxydisulfate (PDS) that was used for removing tetracycline (TC). The catalytic system exhibited good stability, wide pH adaptation, and high resistance to the operational environment. It was supposed that NiN x species could attach to PDS and act as electron acceptors to receive the electrons for activating the PDS, thus generating highly reactive superoxide radicals (⋅O 2 − ) and singlet oxygen ( 1 O 2 ) species for rapid degradation of TC. The electron transfer and dissolved oxygen-derived ⋅O 2 − were also responsible for the degradation of TC. In addition, the Ni@NC-1/PDS system exhibited high efficiency for removing oxytetracycline, ciprofloxacin, or levofloxacin. The results of this study would promote the design of other MOFs-derived carbon-encapsulated metal species for efficiently activating persulfate to remove antibiotics from the wastewater.
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JACS Au
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2021
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IF 0
Yang Wu,Chunlei Pei,Hao Tian,Tao Liu,Xianhua Zhang,Sai Chen,Quan Xiao,Xianhui Wang,Jinlong Gong
The suppression of methane and coke formation over Ni-based catalysts for low temperature ethanol steam reforming remains challenging. This paper describes the structural evolution of Fe-modified Ni/MgAl2O4 catalysts and the influence of iron species on methane and coke suppression for low temperature ethanol steam reforming. Ni–Fe alloy catalysts are gradually oxidized by water to generate Ni-rich alloy and γ-Fe2O3 species at steam-to-carbon ratio of 4. The electron transfer from iron to nickel within Ni–Fe alloy weakens the CO adsorption and effectively alleviates the CO/CO2 methanation. The oxidation capacity of γ-Fe2O3 species promotes the transformation of ethoxy to acetate groups to avoid methane formation and the elimination of carbon deposits for anticoking. Ni10Fe10/MgAl2O4 shows a superior performance with a highest H2 yield of 4.6 mol/mol ethanol at 400 °C for 15 h. This research could potentially provide instructions for the design of Ni-based catalysts for low-temperature ethanol steam reforming.
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CHEMOSPHERE
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2021
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IF 7.086
Fang Zhu,Siyi Zhou,Mengying Sun,Jianfeng Ma,Wei Zhang,Kunjie Li,Hao Cheng,Sridhar Komarneni
Mg doped Ni(OH) 2 was synthesized and investigated as an efficient material to activate persulfate (PS) for phenol degradation. The property of the Ni(OH) 2 material was enhanced by Mg doping as the removal efficiency of phenol was increased from 74.82 % in Ni(OH) 2 /PS system to 89.53 % in Mg-doped Ni(OH) 2 /PS system within 20 min. Such a high removal efficiency revealed that doping Mg into Ni(OH) 2 brings about more defects (oxygen vacancies), which facilitated the formation of more active species in the degradation process. The removal efficiencies of phenol increased with the increase of the initial pH from 3 to 11. The influences of Cl − , NO 3 − and HCO 3 − on the stability of the system were also studied and the results showed that removal rates of all systems in the presence of these different inorganic anions could reached about 90 % within 20 min. Based on the electron spin resonance (ESR) experiments, 1 O 2 , O 2 ·- , ·OH and SO 4 •− were identified as the active species in Mg-doped Ni(OH) 2 /PS system for phenol degradation and a degradation mechanism was proposed for this system. In addition, the as-prepared material retained its activation performance even after 3 repeated cycles.
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NANOTECHNOLOGY
·
2021
·Vol. 32
·期 38
·385602
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IF 3.874
Ximing Zhang,Jingyu Wang,Yang Fan,Hengdong Ren,Zhenying Liu,Yanfen Wang,Yin Liu,Hongcun Bai,Lingbing Kong
In this work, we prepared NiCo alloy/C with rhombic dodecahedron structure and superior microwave absorption performance by using ZIF-67 as the raw material. The rhombic dodecahedron NiCo alloy/C was with rough particles on the surface was photographed by field emission scanning electron microscopy. By adjusting the doping amount of Ni and the temperature of pyrolysis, improved the impedance matching of NiCo alloy/C. Specifically, NiCo alloy/C exhibits a minimum reflection loss of −65.48 dB at 13.48 GHz, while the thickness is 1.63 mm. Defects introduced in the Ni doping process and the special rhombic dodecahedral structure can cause multiple loss mechanisms. Therefore, this NiCo alloy/C composite has the potential to be a potential microwave absorber material with lightweight and high microwave absorption properties.
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WATER RESEARCH
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2021
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IF 11.236
Jia Deng,Enlai Gao,Feng Wu,Zhixiong You,Xiaozhong Li,Shuxian Gao,Li-Zhi Huang
Atomic hydrogen (H•) is highly reactive for the hydrodechlorination of trichloroethylene (TCE). In this work, we found that the coprecipitation of Ni 2+ and Fe 2+ at neutral pH led to an unprecedented catalytic generation of H•. The generated H• effectively dechlorinate TCE to nontoxic ethylene and ethane, and Fe 2+ is the only electron donor. The abundant adsorbed H• produced with a Ni/Fe ratio of 0.4 enhances hydrogen evolution reaction causing a low efficiency for hydrodechlorination. In contrast, the active absorbed H• is generated in the crystal lattice of Ni-Fe hydroxides with a Ni/Fe ratio of 3.0 causing highly efficient hydrodechlorination of TCE. This work not only reveals the mechanism of catalytic hydrodechlorination by Ni-Fe hydroxides at neutral pH, but also provides a novel approach to detoxify TCE in contaminated water using facile precipitated Ni-Fe hydroxides.
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SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Lingyue Liu,Peng Zhou,Xiaozhi Su,Yuhang Liu,Yuhan Sun,Hongbin Yang,Heyun Fu,Xiaolei Qu,Shantang Liu,Shourong Zheng
Monitoring sulfur dioxide (SO 2 ) in the environment requires a sensor to feature adequate sensitivity, selectivity, and low detection levels. Herein, we report an ultrasensitive, low-concentration SO 2 gas sensor that employs single atoms nickel anchored on oxygen vacancy-rich SnO 2 nanorods (SAC-Ni/H-SnO 2 ) as the sensing material. The response value of the SAC-Ni/H-SnO 2 sensor to 20 ppm SO 2 is 48, and the detection limit is 100 ppb, which is superior to most of reported SO 2 sensors. In-situ DRIFTS and ESR characterization shows that the coupling effects of SAC-Ni and adjacent oxygen vacancy on SnO 2 surface, which promote the adsorption of SO 2 and activation of chemisorbed oxygen, respectively. This effective single-atom catalyst provides a new insight into complex gas sensing mechanisms and demonstrates a promising approach of using single-atom catalysts for gas sensing applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Kang Li,Chunlei Pei,Xinyu Li,Sai Chen,Xianhua Zhang,Rui Liu,Jinlong Gong
The modulation of the interaction between the active metal and the underlying support material plays a key role and remains a challenge in many important catalytic reactions. This paper describes a new method for the modification of Ni/Al 2 O 3 by La 2 O 2 CO 3 , which is responsible for modulating the interaction between Ni and the Al 2 O 3 support. When La 2 O 2 CO 3 is loaded on the Al 2 O 3 support as a La 2 O 3 precursor, combined with XRD, H 2 -TPR, H 2 -pluse chemisorption, Raman spectroscopy and TEM characterization, it is found that La 2 O 2 CO 3 can prevent Ni from entering the alumina support and forming NiAl 2 O 4 . This strategy allows more Ni to be reduced and exposed as active sites. Consequently, the La 2 O 2 CO 3 modified Ni/Al 2 O 3 exhibited superior activity with respect to the reference La 2 O 3 modified Ni/Al 2 O 3 and original Ni/Al 2 O 3 in dry reforming of methane (DRM). At the same time, La can cover the acidic sites of alumina and increase the alkalinity of the catalyst, thereby promoting carbon dioxide adsorption and activation, and inhibiting carbon deposition. In addition, the introduction of La also inhibits the sintering of Ni under harsh reaction conditions by enhancing the interaction between Ni metal and the support. This modification method can simultaneously improve the reactivity and stability of the catalyst by altering the interaction between the metal and the support.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2019
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IF 3.218
Na Wang,Gaoyi Han,Hua Song,Yunzhen Chang,Wenjing Hou,Yaoming Xiao
The flexible supercapacitors (FSCs) have attracted much attention with the development of personal electronics. Here, the polyethylene-polypropylene fibrous membranes (PE-PPFMs) are used as the substrate to prepare conductively metallized organic films (Ni/PE-PPFMs) by employing electroless nickel plating method. After graphene oxide (GO) dispersion is coated on the substrate of Ni/PE-PPFMs, electrochemical reduction is carried out to reduce GO and the electrodes of ErGO/Ni/PE-PPFMs have been obtained. The preparation conditions have been optimized and the electrodes have also been characterized in detail. The capacitive performances of the electrodes are evaluated by assembling the FSCs with the NaOH/polyvinyl alcohol (NaOH/PVA) as the gel electrolyte. The specific capacitance of the optimized electrode can reach 368.2 mF cm −2 (147.3 F g −1 based on the active materials), and the maximum energy density of the cell can reach 16.2 μWh cm −2 (or 3.2 Wh kg −1 ) when the power density is 0.24 mW cm −2 (48 W kg −1 ). Meanwhile, the cell exhibits excellent cyclic stability (the capacitance retention can still keep at 89.5% after 10,000 cycles) and flexibility (84.4% capacitance retention after 5500 bending cycles). This strategy provides a simple and environmentally friendly method to prepare flexible rGO-based electrodes.
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Sustainable Energy & Fuels
·
2019
·Vol. 4
·期 1
·164-170
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IF 4.912
Shijian Luo,Xiaoman Li,Wanguo Gao,Haiqiang Zhang,Min Luo
Today, industrial ammonia synthesis mainly depends on the Haber–Bosch process, which causes a lot of energy consumption and huge CO2 emissions. The electrochemical N2 reduction reaction (NRR) is considered a more sustainable and environmentally benign alternative to produce ammonia, but it requires an efficient catalyst to overcome the difficulty of N2 activation. In this work, we reported that MOF-derived C@NiO@Ni microtubes behaved as a high-efficiency electrocatalyst in 0.1 M KOH electrolyte. This electrocatalyst achieved a high NH3 yield of 43.15 μg h−1 mgcat.−1 and faradaic efficiency of 10.9% at −0.7 V vs. a reversible hydrogen electrode. The experimental results indicated that the excellent NRR performance originated from the oxygen vacancies in NiO. Moreover, the abundant NiO/Ni interfaces were conducive to proton adsorption and further enhanced the NRR performance.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Jie Zhu,Guolin Cao,Yunjiao Li,Shilei Wang,Shiyi Deng,Jia Guo,Yongxiang Chen,Tongxing Lei,Jinping Zhang,Shenghong Chang
The transition metals in ternary oxide cathode materials for lithium-ion batteries inevitably exchange with protons in LiPF 6 -containing electrolytes to be dissolved, leading to loss of the active material and rapid capacity fading. Here, a chemically inert Nd 2 O 3 interlayer is employed to avoid the direct contact of the active material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) and electrolyte. As a result, Nd 2 O 3 -coated LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) shows improved cycle performances with a capacity retention of 88.0% after 100 cycles over 3.0–4.4 V, 9.3% higher than the retention of the bare NCM811. Even at an elevated temperature, Nd 2 O 3 -coated NCM811 exhibits better cycle performance as well. The superior electrochemical performances for Nd 2 O 3 -coated NCM811 are ascribed to that Nd 2 O 3 encapsulation-assisted surface passivation alleviates the undesirable interface side reactions and transition metal dissolution (TMD). These features suggest the promising potential of chemically inert Nd 2 O 3 as a long-acting surface modifier in passivating electrolyte/electrode interface.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Hongjie Yu,Ziqiang Wang,Shuli Yin,Chunjie Li,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
As a promising alternative approach to industrial N2 fixation process, electrocatalytic N2 reduction reaction (NRR) can achieve efficient, sustainable, and eco-friendly ammonia production under ambient conditions. Developing efficient NRR catalysts is critical for the electrochemical ammonia synthesis. Herein, self-supported mesoporous Au3Pd film on Ni foam (mAu3Pd/NF) has been in situ synthesized via a micelle-assisted replacement strategy. Combination of bimetallic compositions, interconnected mesoporous structure, and binder-free characteristic, the mAu3Pd/NF shows a superior NRR performance in 0.1 M Na2SO4. This micelle-assisted replacement route is very important to construct efficient self-supporting mesoporous films for the NRR and other fields.
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ACS Catalysis
·
2019
·
IF 12.221
Fei Xiao,Xueping Qin,Mingjie Xu,Shangqian Zhu,LiLi Zhang,Youngmin Hong,Sang-Il Choi,Qiaowan Chang,Yuan Xu,Xiaoqing Pan,Minhua Shao
Thermal annealing is commonly used to remove surface contaminants and redistribute elements in alloys. In this study, Pt–Ni alloy nanoparticles supported on carbon black are selected as a model catalyst to understand the relationship between the annealing conditions (temperature and atmosphere) and the electrocatalytic performance for oxygen reduction, hydrogen evolution, and ethanol oxidation reactions. The impacts of thermal treatment temperature and atmosphere on structures, compositions, and in turn electrocatalytic activities are systematically studied. Interestingly, an ultrathin carbon layer can be formed on the nanoparticle surface by heat treatment in Ar atmosphere at temperatures higher than 350 °C, which significantly decreases its activity toward oxygen reduction and ethanol oxidation reactions. This carbon coating, however, is absent in other atmospheres including N2, air, 7% H2/Ar, and vacuum. Aberration-corrected scanning transmission electron microscopic characterizations with atomic-level resolutions confirm the formation of a Ni-enriched surface on Pt–Ni/C after treatment in Ar, which plays a critical role in catalyzing the growth of stable carbon layers from the surrounding carbons. Further density functional theory calculation results suggest that the absence of a carbon layer in N2 may originate from the stable N–C bond formed during heat treatment and passivation effect of adsorbed N2. It illustrates different effects of inert gases on carbon layer formation by combining experimental and computational approaches. These results may shed light on the proper design of postheat treatment protocols for carbon-supported catalysts and may also provide a feasible method to coat carbon layers on nanoparticle surfaces for various energy storage and conversion applications.
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