INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Jie Guo,Yongjiang Hou,Bo Li,Yulei Liu
Ni–Co–B hollow nanospheres were synthesized by the galvanic replacement reaction using a Co–B amorphous alloy and a NiCl 2 solution as the template and additional reagent, respectively. The Ni–Co–B hollow nanospheres that were synthesized in 60 min (Ni–Co–B-60) showed the best catalytic activity at 303 K, with a hydrogen production rate of 6400 mL hydrogen min −1 g catalyst −1 and activation energy of 33.1 kJ/mol for the NaBH 4 hydrolysis reaction . The high catalytic activity was attributed to the high surface area of the hollow structure and the electronic effect. The transfer of an electron from B to Co resulted in higher electron density at Co sites. It was also found that Ni was dispersed on the Co–B alloy surface as result of the galvanic replacement reaction. This, in turn, facilitated an efficient hydrolysis reaction to enhance the hydrogen production rate. The parameters that influenced the hydrolysis of NaBH 4 over Ni–Co–B hollow nanospheres (e.g., NaOH concentration, reaction temperature, and catalyst loading) were investigated. The reusability test results show that the catalyst is active, even after the fifth run. Thus, the Ni–Co–B hollow nanospheres are a practical material for the generation of hydrogen from chemical hydrides .
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ACS Omega
·
2018
·
IF 0
Changhui Zhu,Qiying Liu,Dan Li,Haiyong Wang,Caihong Zhang,Chunhua Cui,Lungang Chen,Chiliu Cai,Longlong Ma
Crystal α-zirconium phosphate (α-ZrP) was prepared by a hydrothermal method and exfoliated into a layered structure by n-hexylamine (C6H13NH2). Ni-based catalyst (Ni/ZrP) was promoted by loading nickel on the layered α-ZrP via ion exchange. The catalyst was performed to catalyze hydrodeoxygenation of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF), and a 68.1% yield of DMF and 100% conversion of HMF were achieved at 240 °C, 5 MPa H2, and 20 h. The DMF yield can still retain 52.8% after five cycles. The characteristics of the catalyst were investigated via N2 adsorption–desorption, X-ray diffraction, field emission scanning electron microscopy, high-resolution transmission electron microscopy, pyridine-adsorbed Fourier transform infrared (FTIR) spectra, FTIR spectra, inductively coupled plasma mass spectrometry, and thermogravimetric analysis–mass spectrometry, as well as Raman spectroscopy. A pathway from HMF to DMF was found with MF as the intermediate product, and DMF production was preferable via the −CH2OH group hydrogenolysis of HMF over Lewis acidic sites of Ni/ZrP, which is caused by the zirconium vacant orbits.
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PubMed
Energy Technology
·
2018
·Vol. 7
·期 3
·1800694
·
IF 3.175
Chen Zhu,Jing-Pei Cao,Tao Xie,Xiao-Yan Zhao,Xin Cui,Zhen-Xing Guo,Wen-Zhong Shen,Jin Bai,Xian-Yong Wei
The influence of the type of support [activated carbon (AC), HZSM-5, and γ-Al 2 O 3 ] on the performance of Ni-based catalysts for the catalytic hydrogenolysis (CH) of benzyl phenyl ether (BPE) is investigated. The properties of an Ni-based catalyst are investigated using diverse characterization techniques. An Ni/AC catalyst exhibits the highest dispersion of Ni atoms by CO pulse. The kinetic studies show that the apparent activation energies ( E a ) for CH of BPE increase in the order E a (Ni/AC) < E a (Ni/γ-Al 2 O 3 ) < E a (Ni/HZSM-5), and the initial turnover frequencies follow the order of Ni/AC (64 mol mol Nisurf −1 h −1 ) > Ni/γ-Al 2 O 3 (58 mol mol Nisurf −1 h −1 ) > Ni/HZSM-5 (45 mol mol Nisurf −1 h −1 ). All these results prove that the CH activity of BPE is significantly affected by the type of support, and Ni/AC is the highest activity catalyst in CH of the C—O bond of BPE. Toluene and phenol are major products in CH of BPE at a relatively low hydrogen pressure and high temperature. Based on catalytic experiments, a reaction mechanism is proposed, which provides the theoretical basis for converting lignite into high-value organic molecules.
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Energy Technology
·
2019
·Vol. 7
·期 10
·1900649
·
IF 3.163
Yiqun Du,Shimeng Zhao,Cheng Xu,Wenyang Zhang,Pan Li,Huixin Jin,Youjian Zhang,Zihan Wang,Jianxin Zhang
Rechargeable aluminum batteries (RABs) have been intensively studied recently in virtue of high volumetric energy density and cheapness. However, limited options for suitable cathode materials is the major obstacle to their large-scale application. Herein, nickel-iron layered double hydroxide (NiFe–LDH) microspheres with reduced graphene oxide (rGO) are reported as cathode for RABs. It is demonstrated that NiFe–LDH can provide large interlayer spacing for aluminum ions to interact, and the introduction of rGO endows NiFe–LDH with excellent structure stability, electronic conduction, and electrochemical reaction kinetics. The aluminum battery with a NiFe–LDH/rGO cathode delivers a high reversible capacity of 131 mA h g −1 at 1 A g −1 with nearly 100% coulombic efficiency after 100 cycles. The characterization results reveal that the reversible Al 3+ insertion/extraction along with the multielectron redox reactions occurs in the NiFe–LDH/rGO during the cycling process. The aforementioned strategies shed new light on the selection of compatible cathodes for RABs.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Wei Xia,Gui-Zhi Guo,Xue-Qian Wu,Ya-Meng Yin,Ya-Pan Wu,Shuang Li,Ruan Chi,Dong-Sheng Li
Direct methanol fuel cells (DMFCs) can permit the utilization of noble-metal-free electrocatalysts , which certainly reduces the cost and accelerates their practical implementation. With the exploration of efficient and economical methanol oxidation reaction (MOR) catalysts, Ni-based nanostructures have been recognized as the most promising MOR catalysts in alkaline media. Herein, we construct a novel heterojunction MOR electrocatalyst composed of Ni-based metal-organic framework (Ni-MOF) and NiFe-based layered double hydroxides (LDHs) through a coordination-induced self-assembly strategy. Owing to the synergic effect between Ni and Fe sites, coupled with the effect of hetero-interface, the resultant Ni-MOF/NiFe-LDH composite exhibits remarkable MOR activity in 0.1 M KOH electrolyte with the oxidation current density (32.66 mA cm −2 ) is 2.65 and 2.44 times higher than that of the primitive NiFe-LDH and Ni-MOF. The excellent stability of the Ni-MOF/NiFe-LDH electrocatalyst has also been confirmed by long-term chronoamperometry (CA) analysis. Our work paves a facile controllable way for fabricating MOF/LDH heterostructure targets on MOR and underlines its potential to boost energy conversion efficiency through the manipulation of synergic components.
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Materials Chemistry Frontiers
·
2024
·
IF 6
Xin Fu,Bo Pu,Li Pan,Ruiqi Ming,Qian Lv,Xiaobo Chen,Lihong Tian
Urea oxidation reaction (UOR) is a promising substitution for the oxygen evolution reaction (OER) on anode for highly efficient H2 production. However, the sluggish kinetics and high oxidation potential of NiII → NiIII severely limit the activity of Ni-based catalysts in the electrochemical UOR. Herein, composition regulation was adopted to enhance the electrocatalytic activity of a nickel-benzene dicarboxylate framework (Ni-BDC MOF)-derived electrode towards urea oxidation. In 1 M KOH with 0.33 M urea solution, the derived amorphous tri-metallic hydroxide layer on the surface of the NiMnCo MOF, induced by electro-activation, exhibited a low onset potential and a steeply rising current density with increasing applied potential. It achieved a benchmark current density of 10/100 mA cm−2 at an anode potential of 1.28/1.33 V vs. RHE, respectively. In particular, a 500 mA cm−2 current density was reached at an impressively low potential of 1.41 V vs. RHE. This exceptional performance is ascribed to the fact that the open framework provides a large electrochemical active surface, while the multicomponent synergy decreases the NiII → NiIII oxidation potential, enhances electron transfer and promotes the UOR kinetics. This study suggests that rational composition regulation is a promising approach to improving the performance of Ni-based MOF materials towards electrocatalytic urea oxidation.
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AICHE JOURNAL
·
2025
·
IF 4
Bin Chen,Xingwen Cha,Xuexue Dong,Juanjuan Bian,Jiale Huang,Qingbiao Li,Xiaoqing Huang,Guowu Zhan
Upgrading biomass-derived fatty acids through the H 2 -free and solvent-free catalytic deoxygenation process is both safe and eco-friendly. Herein, we used modified rice husk-derived biochar with ultra-high specific surface area and abundant surface groups as a support to design a homologous bimetallic site catalyst containing Ni single atoms (Ni 1 ) and Ni nanoclusters (Ni n ), the synergy between which is dedicated to excellent catalytic performance. The designed catalyst, Ni 1+n /A-bio-AC, demonstrated an impressive 89.8% selectivity for odd-numbered long-chain alkanes during the H 2 -free and solvent-free deoxygenation of stearic acid, with a turnover frequency value over 18 times higher than conventional Ni/AC. Multiple characterizations revealed the coexistence of Ni 1 and Ni n on the catalyst support. Experimental and theoretical calculations showed that Ni n facilitates the adsorption of fatty acid substrates. While Ni 1 serves as highly dispersed Lewis acid sites, enhancing the dehydrogenation of fatty alcohol intermediates during the in situ hydrodeoxygenation and lowering the decarboxylation pathway energy barriers via electronic synergy with Ni n , thus remarkably boosting the catalytic deoxygenation activity. This work provides a novel Ni dual-site catalyst for developing biomass resource conversion technologies.
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ADVANCED MATERIALS
·
2024
·
IF 27.4
Haocheng Ji,Junxiong Wang,Haotian Qu,Junfeng Li,Wenhai Ji,Xiao Qiu,Yanfei Zhu,Hengyu Ren,Ruyu Shi,Guanjun Ji,Wenguang Zhao,Guangmin Zhou
Facing the resource and environmental pressures brought by the retiring wave of lithium-ion batteries (LIBs), direct recycling methods are considered to be the next generation's solution. However, the contradiction between limited battery life and the demand for rapidly iterating technology forces the direct recovery paradigm to shift toward “direct upcycling.” Herein, a closed-loop direct upcycling strategy that converts waste current collector debris into dopants is proposed, and a highly inclusive eutectic molten salt system is utilized to repair structural defects in degraded polycrystalline LiNi 0.83 Co 0.12 Mn 0.05 O 2 cathodes while achieving single-crystallization transformation and introducing Al/Cu dual-doping. Upcycled materials can effectively overcome the two key challenges at high voltages: strain accumulation and lattice oxygen evolution. It exhibits comprehensive electrochemical performance far superior to commercial materials at 4.6 V, especially its fast charging capability at 15 C, and an impressive 91.1% capacity retention after 200 cycles in a 1.2 Ah pouch cell. Importantly, this approach demonstrates broad applicability to various spent layered cathodes, particularly showcasing its value in the recycling of mixed spent cathodes. This work effectively bridges the gap between waste management and material performance enhancement, offering a sustainable path for the recycling of spent LIBs and the production of next-generation high-voltage cathodes.
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PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 110
·90904-90912
·
IF 3.84
Yueling Cao,Junwei Wang,Maoqing Kang,Yulei Zhu
Hydrogenolysis of glucose and cellobiose, used as the model feedstocks, over Ni–WO3/SBA-15 catalysts has been investigated to probe the influencing factors for the conversion of cellulose to ethylene glycol (EG). The conversion of glucose and cellobiose to EG showed different dependencies on reaction temperature; a lower reaction temperature was needed for the former. Additionally, the surface atomic ratio of W to Ni on the Ni–WO3/SBA-15 catalysts was the key factor for the product distribution. Both glucose and cellobiose had their own optimum W–Ni ratio for the production of EG, and the ratio of W to Ni for glucose was slightly lower than that of cellobiose. On the other hand, the Ni–WO3/SBA-15 catalysts were thoroughly characterized by N2 adsorption–desorption, X-ray diffraction (XRD), hydrogen-temperature programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). The results indicated that the reducibility of Ni–WO3/SBA-15 catalysts with high Ni loading was more similar to that of pure NiO. More importantly, the change of surface atomic content of Ni and W of Ni–WO3 catalysts with various Ni loadings resulted from the surface W species of the catalysts being gradually covered by Ni species with the increase of Ni loading.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Chunmin Zhang,Chunli Wang,Qingyun Shi,Xiaoli Wang,Shaolei Zhao,Long Liang,Qingshuang Wang,Limin Wang,Yong Cheng
The high hydrogen release temperature and thermodynamic stability of the coordination hydride LiAlH 4 render it unsuitable for direct application. This work intends to improve the hydrogen release properties via compositing LiAlH 4 and AlH 3 with similar initial hydrogen release temperatures and introduce efficient additive Ni/CeO 2 composite. The thermal stability of the composite system LiAlH 4 -AlH 3 is enormously reduced compared to that of LiAlH 4 . In addition, the preferential release of hydrogen from LiAlH 4 in the composite system provides additional heat for the subsequent release of hydrogen from AlH 3 , accelerating the hydrogen release process. As a result, LiAlH 4 -AlH 3 -Ni/CeO 2 composite performs enhanced hydrogen release performance with a hydrogen release capacity of 8.27 wt% hydrogen within 300 ℃ and a dehydrogenation onset temperature as low as 72.9 ℃. The enthalpy change of the first step hydrogen release reaction decreases from −11.99 kJ mol −1 (LiAlH 4 ) to −2.02 kJ mol −1 (LiAlH 4 -AlH 3 ). Theoretical calculations indicate that both atomic dehybridisation and electron redistribution expedite the breaking of the Al-H bond and the consequent release of hydrogen.
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RSC Advances
·
2016
·Vol. 6
·期 56
·51221-51228
·
IF 3.289
Yanliang Yang,Jiping Ma,Xiuquan Jia,Zhongtian Du,Ying Duan,Jie Xu
Al2O3 modified by alkaline earth metals M–Al2O3 (M = Mg, Ca, Sr, Ba) was synthesised by coprecipitation method. The nickel-based catalysts supported by M–Al2O3 were prepared by impregnation method. The catalysts were characterized by TEM, N2 adsorption/desorption, XRD, H2-TPR, NH3-TPD and XPS, and used for the direct hydrogenation of furfural to tetrahydrofurfuryl alcohol (THFA) in water. The reaction was demonstrated to proceed through furfuryl alcohol as an intermediate. The modification of Al2O3 by alkaline earth metals has a significant effect on the activity and selectivity of THFA. A high yield of THFA was obtained over Ni/Ba–Al2O3 under optimized conditions. Moreover, the catalyst is recyclable and reusable at least four times without significant loss of the conversion of furfural and selectivity of THFA.
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ELECTROCHIMICA ACTA
·
2016
·
IF 4.803
Hongyan Chen,Xing Chang,Daming Chen,Jinbao Liu,Ping Liu,Yuan Xue,Hualin Lin,Sheng Han
A hierarchically flower-like structure with nanoarrays coupled with 3D macroporous sponge graphene combines the preponderances of the hierarchical nanoarchitecture and composition to enhance electrochemical performance. A graphene-karst cave flower-like Ni-Mn layered double oxides (GL) electrode material was prepared through a mild hydrothermal-carbonization process. As an electrode material, the resulting GL composite exhibited excellent performance with high specific capacitance (1,648 and 1,252 F g −1 at 0.5 and 10 A g −1 , respectively) and good cycling stability (almost 96% retention after 6,000 charge-discharge cycles) for energy storage electrode. The GL composite material acting as a positive electrode for the asymmetric supercapacitor also exhibited high specific capacitance of 116.56 F g −1 at 0.5 A g −1 and excellent cycling stability with 86.7% capacitance retention after 6,000 cycles at a current density of 5 A g −1 . This outstanding electrochemical performance may be attributed to the synergistic effect of the layered double oxides and 3D macroporous graphene oxide sponge.
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