ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Chao Miao,Kaixuan Shang,Lixing Liang,Shumei Chen,Jing Ouyang
In this work, a Ni-based catalyst supported on a core–shell structure catalytic carrier material (Ni/ZSM-5@MCM-41) based on kaolinite tailings is reported, which exhibits excellent CO2 methanation performance at atmospheric pressure. At 400 °C, CO2 conversion and CH4 selectivity reach 80 and 97% with the space velocity of 12,000 mL gcat–1 h–1, respectively, and it can maintain good stability during the 80 h stability test. Compared with traditional Ni/ZSM-5 and Ni/MCM-41 catalysts, Ni/ZSM-5@MCM-41 has more substantial confinement effects on the active components, and the active components are more evenly dispersed on surface of the carrier. In addition, it is confirmed by the in situ diffuse reflectance infrared Fourier transform spectroscopy technique that CO2 methanation over the Ni/ZSM-5@MCM-41 catalyst follows the path of formate and CO as intermediates.
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ACS Applied Nano Materials
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2022
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IF 6.14
Jiandan Chen,Guangxian Liu,Qi Xiao,Chenwei Wang,Zhenzeng Zhou,Chunchuan Gu,Zheng-Zhi Yin,Hongying Liu
Glucose concentration in the body is a very important index for health evaluation. Nonenzymatic glucose biosensors attract persistent interest and research. The acupuncture technique has been developed for treating the disease for thousands of years. Here, a stainless-steel acupuncture needle (AN) was first used to sense glucose after functionalizing with bimetal of gold nanoparticles (AuNPs) and nickel nanoparticles (NiNPs). AuNPs were electrodeposited as particle clusters, and the NiNPs could be further electrodeposited around AuNPs to form a nano-pinecone shape with a size of about 600 nm. Au/AN exhibited the best electroconductivity compared to the weakest Ni/AN and medium Ni/Au/AN interfaces. Three nanotechnically processed interfaces showed obvious electrochemical response behavior for glucose compared with the bare AN. Surprisingly, the matrix of AuNPs could drastically boost the electrochemical response of NiNPs for glucose, which might be due to the abundance of active sites in the bimetallic hierarchy. The Ni/Au/AN electrode possessed an additive signal compared with Au/AN and Ni/AN. Under the optimized conditions, the prepared nonenzymatic biosensor exhibited two linear relationships in the wide concentration range of 0.5 μM to 1.5 mM and 1.5–5 mM with sensitivities of 766.02 and 368.77 (μA/mM/cm2), and the limit of detection was 0.14 μM. Moreover, the Ni/Au/AN showed superior performance over reported electrodes with great selectivity, stability, and reproducibility. The apparent Km of 0.161 mM was lower than that of glucose oxidase, implying that the Ni/Au-modified AN exhibited a strong affinity for glucose. The fabricated biosensor can be successfully used for the detection of glucose concentration in human serum, which provided a leading direction and potential for clinical point-of-care monitoring.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Guangya Hou,Zhongwei Shen,Yiping Tang,Qiang Chen,Huazhen Cao,Huibin Zhang,Guoqu Zheng,Jianli Zhang
Direct methanol fuel cells and direct urea fuel cells are significant for mitigating the energy crisis and protecting the environment. However, as the common critical anodes for the electrooxidation of methanol and urea, most Ni-based catalysts are severely poisoned by the CO group, resulting in a decrease in current densities and stability of fuel cells. Herein, efficient bacterial cellulose (BC)-derived carbon aerogel loaded with Ni-based catalyst and WC nanoparticles co-catalyst was developed for the electrooxidation of methanol and urea. As a result, the catalytic electrode exhibits high electrocatalytic activity for methanol electrooxidation (105.7 mA cm −2 at 0.8 V) and urea electrooxidation (90.4 mA cm −2 at 0.8 V). The synergistic effect between Ni and WC can significantly weaken the surface adsorption of CO on the electrode to obtain excellent and durable electrochemical performance. For methanol oxidation reaction and urea oxidation reaction, the retentions of the peak current density after 2000 cycles in the original electrolytes are 48.94% and 74.79%, respectively. Moreover, applying the new electrolyte, the peak current density can return to 88.42% and 84.4% of the original value.
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 9
·2787-2802
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IF 2.936
Shi Yu,Li Yiming,Wang Shiwei,Chu Yuting,Yu Hongbo,Li Tong,Yin Hongfeng
A series of relative inert SiO 2 supported NiP-x/SiO 2 catalysts, containing different ratio of metallic nickel to nickel phosphides, were employed to clarify the synergistic effect of metallic nickel–nickel phosphides in dry methane reforming reaction. Ni/SiO 2 catalyst exhibits good activity but severe carbon deposition and visible nickel particles sintering in dry methane reforming, which results in evident deactivation after 50 h reaction. The presence of P increases the dispersion of nickel species, results in smaller nickel species particles size. The co-existence of metallic nickel and nickel phosphides species was confirmed by multiple characterizations. Because of the relative stronger CO 2 dissociation properties, NiP-x/SiO 2 catalysts exhibit higher resistance of carbon deposition. In addition, P content makes great difference to not only carbon deposition but also activity in dry methane reforming. NiP-3/SiO 2 , which has good activity, stability and anti-coking properties in dry methane reforming, is the optimal catalyst in our study scope. Graphical Abstract
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Shuai Sun,Tianci Wang,Kejiang Qian,Hao Zhang,Kaifeng Ji,Zijian Shi,Mingyu Chen,Cui Zhang,Shuangxi Liu
High-efficiency water splitting catalysts are competitive in energy conversion and clean energy production. Herein, a bifunctional water splitting catalyst CoNiP with cation vacancy defects (CoNiP–V) is constructed through defect engineering. The results show that abundant cation vacancy defects in CoNiP–V are bifunctional active centers in the process of water electrolysis , which enhance the activity of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). In 1.0 mol L −1 potassium hydroxide, CoNiP–V requires a pretty low overpotential of 58 mV to reach a geometrical current density of 10 mA cm −2 for HER. To deliver a current density of 100 mA cm −2 , only 137 mV and 340 mV of overpotential are needed for HER and OER, respectively. Moreover, the cell with CoNiP–V as both cathode and anode exhibits good stability, which only needs 1.61 V to achieve a current density of 100 mA cm −2 , and the cell voltage barely rises 10% after 100 h’ test under 100 mA cm −2 . Therefore, CoNiP–V is promising for the development of efficient water splitting catalysts.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Tangtong Ju,Yue Dai,Hailong Tang,Meiling Wang,Xiao Sun,Min Wang,Yongqing Ma,Ganhong Zheng
Direct conversion of CH 4 to high valued chemicals under mild conditions is attractive but full of challenges. Here, we present a ternary composite that consists of Ni-doped TiO 2 nanocubes (NCs) and CNTs as a new kind of catalyst (denoted as CNTs-Ni@TiO 2 NCs) for CH 4 photocatalytic conversion to C1 oxygenated products at 30 °C. Using H 2 O 2 as an oxidant, a high C1 oxygenated products yield and selectivity of 1.43 mol/(mol Ni ·h) and 95.6% can be reached in 2 h at 30 °C. The superior photocatalytic performance resulted from the synergistic effects of TiO 2 NCs, Ni species, and CNTs such as enhanced visible light absorption , improved electron/hole separation and charge transfer property, and lowered C-H bond cleavage energy required for CH 4 activation, were carefully studied. Good reusability of the catalyst was studied by recycle experiments. Possible reaction mechanism based on the radical routes were carefully discussed by combining in-situ Fourier transform infrared spectroscopy , X-ray photoelectron spectroscopy, electron spin resonance spectroscopy, radical scavenger experiments and density functional theory calculation.
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JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Jinxiao Ba,Hui Cheng,Zhenhan Li,Xianghai Yu,Aiying Song,Chengqun Xu,Donghua Fan,Shengye Jin
In this work, we develop Ni/Ni 3 S 2 /CdS composite photocatalytic system from annealing of CdS nanosphere coated Ni-ZIF by simple solvothermal method. The Ni/Ni 3 S 2 /CdS synthesized after calcination at 700 °C exhibits the best hydrogen evolution performance with an average hydrogen evolution rate of 2104.02 μmol/g/h, which is 152 times higher than that of pure CdS, and external quantum efficiency is 41.9% (λ = 420 nm). Using a series of characterization methods, we revealed that CdS is the photosensitizer, Ni is the catalytic active species, and Ni 3 S 2 formed between Ni and CdS formation plays an important role in charge separation as confirmed by time resolved emission spectroscopy. In addition, the regulation of Ni loading is achieved by changing the annealing time and the molar ratio of Ni salt to CdS. These results demonstrate that Ni/Ni 3 S 2 /CdS is a favorable photocatalyst for efficient photocatalytic hydrogen evolution.
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Nanoscale
·
2022
·Vol. 14
·期 34
·12275-12280
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IF 8.307
Wenxiu Yan,Chao An,Yongli Shen,Shuyuan Zeng,Changhua An
Engineering of the crystal structures of metallic nanomaterials is an alternative avenue to control the size and shape of nanocatalysts. However, the phase-controlled synthesis of Ni nanocatalysts is challenging because of its low reduction potential under mild conditions. We developed a room-temperature CH4 plasma conversion of Ni(OH)2 nanosheets to hexagonal close packed (hcp) Ni while maintaining a pristine shape. Increasing the temperature resulted in the formation of face-centered cubic (fcc) Ni. The hcp Ni nanosheets exhibited an overpotential of 85 mV at 10 mA cm−2 for an electrocatalytic hydrogen evolution reaction (HER) in alkaline solution, which was superior to that of the fcc (122 mV) counterpart. Density-functional-theory calculations demonstrated that during the HER, the d-band center of hcp Ni was closer to the Fermi level, which aided the formation of H2 molecules. This work could facilitate the synthesis of other metastable metals and metallic alloys with high efficiency for various applications.
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ACS Applied Nano Materials
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2022
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IF 6.14
Yunfang Yan,Xuejie Cao,Liangmin Ning,Fei Lin,Wenzhuo Qin,Xin Liu,Wen Gu
The construction of low-cost electrocatalysts with good conductivity, excellent intrinsic activity, and superior stability is crucial for the hydrogen evolution reaction (HER). Herein, we report an outstanding catalyst (Ni0.2Mo0.8N/NiMoP2/MoO2@NC) consisting of NiMo-based nanorod arrays supported on Ni foams for the efficient alkaline HER. It shows an ultralow overpotential of 48 mV and remarkable longevity for over 145 h at 10 mA cm–2 in 1.0 M KOH. The integration of ample compositions is favorable to the formation of heterointerfaces, accelerating electron transfer. The assembly of transition metal nitrides and phosphides fully develops the electrical conductivity of metal materials, which paves the way for superstability. The superior electrocatalytic activities can be attributed to the vital features, including the synergistic effect of Ni0.2Mo0.8N and NiMoP2, good electrical conductivity of MoO2, and corrosion resistance of NC basement. The present work proposes that regulating compositions and hierarchical nanostructures are of significance in developing electrode materials for the HER.
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HIGH PERFORMANCE POLYMERS
·
2022
·
IF 1.73
Hailong Yu,Jinfeng Cui,Haiyin Zhang,Baoping Yang,Junhong Guo,Bo Mu,Zhaohui Wang,Huaming Li,Li Tian
A functionalized cross-linked polyphosphazenes microsphere (Salen-PZN-Ni@DHPP-PTS) was prepared by wrapping Salen-Ni basis polyphosphazenes (Salen-PZN-Ni) with a kind of hybrid flame retardant (DHPP-PTS) to improve the flame retardancy and smoke suppression properties of epoxy (EP) composites. Thermogravimetric analysis showed that the addition of Salen-PZN-Ni@DHPP-PTS greatly improved the thermal stability of the EP composites. The addition of 5 wt% Salen-PZN-Ni@DHPP-PTS remarkably improved the fire safety of EP, which was illustrated by the results of the cone calorimeter. For example, the peak heat release rate and total heat release rate of the EP composites were reduced by 44.2% and 33.1%, respectively. The limiting oxygen index value of 5% Salen-PZN-Ni@DHPP-PTS/EP composite reached 29.8% and UL-94 achieved V-1 rating. In addition, the introduction of Salen-PZN-Ni@DHPP-PTS effectively suppressed the production of toxic CO and other volatiles. Meantime, the synergistic effect between Salen-PZN-Ni and DHPP-PTS was found. The potential flame retardant mechanism of Salen-PZN-Ni@DHPP-PTS is regarded as the synergistic catalytic carbonization effect and the extremely thermally stable components forming. Enhanced fire safety of EP composites by synergistic interaction of various components (nickel and DHPP-PTS) with polyphosphazenes microspheres.
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FUEL
·
2022
·
IF 8.035
Ben Chen,Bowen Hui,Yuting Dong,Qiang Sheng,Xiang Li,Qinglan Hao,Chunjing Liu
The SiO 2 - and MCM-41-supported Ni catalysts were prepared by an incipient wetness impregnation method and their performance in the hydrogenation of liquid organic hydrogen carrier were evaluated using N-ethylcarbazole (NEC) as model compound. Ni particles were mainly located on the external surface of the SiO 2 -supported Ni catalysts. Both Ni particles on the external surface and filled in the mesopores of MCM-41 were found in the MCM-41-supported catalysts. The reduction of surface Ni particles occurred at low temperature (ca. 365 °C), but the complete reduction of Ni particles in the mesopores of MCM-41 required high temperature (ca. 555 °C). The MCM-41-supported Ni particles possessed lower electron densities than the SiO 2 -supported ones. The surface Ni particles showed the same activity in the hydrogenation of NEC, which were more active than those in the mesopores of MCM-41. A correlation between the electron density of Ni particles and their selectivity was observed. The higher the electron density of Ni particles, the higher the selectivity to the fully hydrogenated product (dodecahydro-N-ethylcarbazole) is.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
·
IF 10.753
Xingwen Lu,Wang Xu,Qinghuai Zeng,Weizhen Liu,Fei Wang
Struvite precipitation is a promising strategy for the simultaneous recovery of nitrogen and phosphorus from waste streams. However, waste streams typically contain high amounts of metal contaminants, including Ni, which can be easily sequestered by struvite, but the behavior of Ni during struvite precipitation remains unclear. Thus, this study investigates the influence of Ni concentrations on struvite precipitation. The quantitative X-ray diffraction (QXRD) results revealed that the purity of struvite decreased from 96.6 to 41.1% with the Ni concentrations increased from 0.1–100 mg·L −1 . At lower Ni concentrations of 0.1–1 mg·L −1 , scanning electron microscopy (SEM) showed a roughened surface of struvite crystal, and this was combined with X-ray absorption near edge structure (XANES) data that indicated a stack of Ni-OH and Ni-PO 4 on struvite surface. At Ni concentrations of 10–25 mg·L −1 , Ni primarily crystalized as Ni-struvite (NiNH 4 PO 4 ·6H 2 O), as detected by QXRD. At higher Ni concentrations of 25–100 mg·L −1 , the co-precipitation of amorphous Ni phosphate(s) (e.g., Ni 3 (PO 4 ) 2 ) and Ni hydroxide (e.g., Ni(OH) 2 ) was identified by XANES. Specifically, the X-ray photoelectron spectroscopy (XPS) analysis detected the formation of amorphous Mg hydroxide(s) and phosphate(s) at Ni of 25–100 mg·L −1 . The overall results revealed that Ni formed Ni-OH and Ni-PO 4 on struvite surface at 0.1–1 mg·L −1 , whereas Ni precipitated as separated phases (e.g. Ni-struvite, Ni hydroxide and phosphate) at 10–100 mg·L −1 . The existence of Ni disturbed the crystal growth of struvite and promoted the formation of Ni-struvite, amorphous products during struvite formation.
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