RSC Advances
·
2021
·Vol. 11
·期 53
·33626-33636
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IF 3.361
Leliang Wu,Yiting Lin,Yimin Zhang,Peng Wang,Mingjun Ding,Minghua Nie,Caixia Yan,Shiyao Chen
Alkaline substances could activate peroxymonosulfate (PMS) for the removal of organic pollutants, but relatively high alkali consumption is generally required, which can cause too high pH of the solution after the reaction and lead to secondary pollution. Within this study, PMS activated by a relatively low dosage of Ca(OH)2 (1 mM) exhibited excellent efficiency in the removal of bisphenol S (BPS). The pH of the solution declined to almost neutral (pH = 8.2) during the reaction period and conformed to the direct emission standards (pH = 6–9). In a typical case, BPS was completely degraded within 240 min and followed the kinetics of pseudo-first-order. The degradation efficiency of BPS depended on the operating parameters, such as the Ca(OH)2, PMS and BPS dosages, initial solution pH, reaction temperature, co-existing anions, humic acid (HA), and water matrices. Quenching experiments were performed to verify that singlet oxygen (1O2) and superoxide radicals (O2˙−) were the predominant ROS. Degradation of BPS has been significantly accelerated as the temperature increased. Furthermore, degradation of BPS could be maintained at a high level across a broad range of pH values (5.3–11.15). The SO4−, NO3− did not significantly impact the degradation of BPS, however, both HCO3− and HA inhibited oxidation of BPS by the Ca(OH)2/PMS system, and Cl− had a dual-edged sword effect on BPS degradation. In addition, based on the 4 identified intermediates, 3 pathways of BPS degradation were proposed. The degradation of BPS was lower in domestic wastewater compared to other naturals waters and ultrapure; nevertheless, up to 75.86%, 77.94% and 81.48% of BPS was degraded in domestic wastewater, Yaohu Lake water and Poyang Lake water, respectively. Finally, phenolic chemicals and antibiotics, including bisphenol A, norfloxacin, lomefloxacin hydrochloride, and sulfadiazine could also be efficiently removed via the Ca(OH)2/PMS system.
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ACS Catalysis
·
2021
·
IF 13.084
Jinqiu Guo,Zongjing Feng,Jun Xu,Jie Zhu,Guanghui Zhang,Yaping Du,Hongbo Zhang,Chunhua Yan
Ethanol transformation with high product selectivity is a great challenge, especially for high weight molecules. Here, we show a combination study of kinetic, thermodynamic, and in situ spectroscopy measurements to probe the selective upgrading of ethanol over lamellar Ce(OH)SO4·xH2O catalysts, with 60–70% Ce3+ preserved during the catalysis. High methyl phenols (MPs) selectivity at ∼80% within condensation products was achieved at ∼50% condensation yield (3.0 kPa C2H5OH, 15 kPa H2, Ar balanced, 693 K, 1 atm, gas hourly space velocity (GHSV) ∼5.4 min–1), with acetaldehyde, acetone, 4-heptanone, and 2-pentanone as the key reaction intermediates. Kinetic measurements with the assistance of isotope labeling proved that MPs generated from the kinetically relevant step (KRS) of C–C bond coupling of enolate nucleophilically attacks surface C2H4O following a Langmuir–Hinshelwood model. Low ethanol and water pressures and high acetaldehyde and hydrogen pressures were proved to be favored for MPs generation rather than dehydration, in which hydrogen could reduce the amount of lattice oxygen and facilitate the preparation of MPs while water and ethanol both compete with acetaldehyde for active sites during catalysis. On the basis of in situ X-ray diffraction (XRD), quasi-in situ X-ray photoelectron spectroscopy (XPS), and Raman characterizations, the Ce(OH)SO4 crystal structure was proved to be maintained along with ethanol activation, and the Ce3+–OH Lewis acid–base pair was proved to be the active species for the selective C–C bond coupling. The KRS assumption was also supported by the apparent activation energy assessment within the reaction network on dehydration, dehydrogenation, aldol condensation, and cyclization and a series of negligible kinetic isotope effects (KIEs). This system can be easily extended to some other systems related to C–C bond coupling and is attracting attention on converting oxygenate platform molecules over lanthanide species.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2021
·
IF 8.067
Guanglu Li,Chang Liu,Zhao Zhang,Baihua Cui,Yanan Chen,Yida Deng,Wenbin Hu
Oxygen evolution and oxygen reduction are considered as essential processes in the energy conversion devices. The progress of cost-effective bifunctional catalysts has become a critical issue to be solved. Here, we report that Co(OH) 2 @N-doped carbon (NC) was facilely synthesized through the impregnation strategy of metal-organic frameworks derived carbon and cobalt ions. N-doped carbon with porous structure and cobalt hydroxide nanosheets play a synergistic effect role, representing excellent catalytic performance toward oxygen evolution and reduction reactions. The obtained Co(OH )2 @NC exhibits remarkable activity in terms of a lower overpotential of 330 mV@10 mA cm −2 for OER and a more positive half-wave potential (E 1/2 = 0.84 V) for ORR in alkaline medium, outperforming IrO 2 and Pt/C. Due to its superior bifunctional catalytic performance, Co(OH) 2 @NC catalyst is applied into a promising air electrode of Zn-air battery. This presented strategy of impregnation synthesis in this work provides a new design direction for practical electrochemical energy devices.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2020
·
IF 5.647
Shuo Li,Jia Liu,Tianwei Tan,Jiapei Nie,Huili Zhang
To reduce the emission of greenhouse gases, the substitution of fossil fuel by renewable energy sources is increasingly important. Matching energy supply and demand is however required, even more so if intermittent renewable energy sources are employed. Thermal energy storage then offers significant advantages. Thermo-chemical energy storage systems, using reversible reactions, have a high reaction enthalpy that exceeds the storage capacities of sensible and latent heat modes. Magnesium hydroxide is a candidate TCES material for such a system at temperature around 300 °C, and adaptable when doping Mg(OH) 2 with metal salts. Both pure Mg(OH) 2 and its composites with 1, 3, 6 and 10 wt% LiNO 3 are studied. The present work validates this TCES process and develops reaction rate equations needed for its design. The LiNO 3- doping significantly reduces the onset temperature of dehydration. For pure Mg(OH) 2 , the temperature is 325 °C. It is reduced to 289 °C when 1 wt% LiNO 3 is present, and further reduced to 269 °C at a dosage of 10 wt% LiNO 3 . Whereas the dehydration of pure Mg(OH) 2 is slow, with a rate constant k of 1.72 10 −5 s −1 at 300 °C, adding increasing amounts of LiNO 3 progressively increases the reaction rate constant to ~10 −2 s −1 at 300 °C when 10 wt% LiNO 3 is present. The kinetic expressions enable to predict the conversion yield and amount of heat stored or released for any desired temperature and selected duration of the heat-induced dehydration. LiNO 3- doped Mg(OH) 2 have a high potential in TCES applications when the heat source is available at temperatures between 250 and 400 °C, since the equilibrium temperature and the extent of de-hydration Mg(OH) 2 can be tuned to the required temperature range by adding different wt% of LiNO 3 .
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
·
IF 3.99
Bin Yan,Ji Lan,Yueshan Li,Yinjie Peng,Lingying Shi,Rong Ran
In this paper, hexagonal Ni(OH) 2 nanosheets were prepared by hydrothermal method with nickel chloride hexahydrate as matrix and ammonia as precipitant. The lateral size of Ni(OH) 2 nanosheets was about 100–250 nm. The structure of the Ni(OH) 2 sheets was characterized by XRD , SEM , IR, TGA etc. Pickering emulsion was prepared by using Ni(OH) 2 nanosheets as stabilizer and dichloromethane (DCM) as oil phase. Furthermore, the stability factors of Pickering emulsion and the adsorption of Congo red (CR) on interface particle layer were studied. The adsorption equilibrium of CR was analyzed by Langmuir adsorption model and Freundlich adsorption model, and the adsorption process was researched by pseudo-first-order kinetics and pseudo-second-order kinetics. Compared with Ni(OH) 2 in the water phase, the Ni(OH) 2 in interface particle layer exhibited a much higher adsorption capacity and a faster deposition rate . The adsorption mechanism of CR can be mainly attributed to electrostatic interaction between the positively charged interface particle layer and the anionic CR molecules. It can be expected that as a promising adsorbent for CR removal in water treatment, the Ni(OH) 2 sheets in Pickering interface layer can provide a new strategy for dye adsorption.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Xianshu Qiao,Hongjun Kang,Yang Li,Kai Cui,Xin Jia,Henghao Liu,Wei Qin,Max Pupucevski,Gang Wu
We report a highly efficient and stable electrode composed of a porous Fe-doped β-nickel hydroxide nanopyramid array supported on nickel foam (U–Fe-β-Ni(OH)2/NF) for overall water splitting. The unique structure is assembled via a self-templated strategy by utilizing the FeNi oxalate (FeNi–C2O4/NF) nanopyramid as the templates, followed by an anion-exchange reaction at room temperature. Due to the intrinsic activity of Fe-doped β-Ni(OH)2 along with unique porous array structures consisting of two-dimensional (2D) active materials on three-dimensional (3D) conductive substrates, the developed electrode exhibited outstanding electrocatalytic activity for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in an alkaline medium. The introduced amount of Fe plays a significant role in promoting OER and HER activity compared to the β-Ni(OH)2 electrode. The optimal electrode (U–Fe-β-Ni(OH)2/NF-2) generated a current density of 10 mA cm–2 at low overpotentials of 218 mV for the OER and 121 mV for the HER. The electrode also demonstrated considerably stable performance during the continuous water splitting process. Furthermore, we elucidated the promotion mechanisms of the active Fe-doped β-Ni(OH)2 compound for the OER and HER based on extensive characterization and electrochemical measurements. Hence, this work provides a facile approach to developing low-cost, efficient, and stable hydroxide-based electrodes for bifunctional OER and HER in water splitting.
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JOURNAL OF POWER SOURCES
·
2026
·
IF 8.4
Qian-Yu Wang,Sian-Hong Ong,Zi-Ye Liu,Zhong-Wei Zhang,Quan-De Li,Ji-Ming Hu
Conductive graphene nanosheets boost oxygen evolution electrocatalysis. • Electrochemically assisted deposition forms porous Ni(OH) 2 /NiO onto freestanding graphene. • Low overpotential of 260 mV at 10 mA cm −2 and Tafel slope of 41 mV dec −1 . • Macroscopic model indicates faster *OOH formation with transfer coefficient of 0.74 Developing low-cost oxygen evolution reaction (OER) catalysts with efficient charge transport and accessible active sites is essential for alkaline water electrolysis. Here we report an electrochemically assisted technique (EAT) to deposit highly dispersed Ni(OH) 2 species on the surface of freestanding graphene (Gr) without deliberate surface functionalization, where a transient SiO 2 -derived framework assists the deposition process of Ni(OH) 2 , followed by heat treatment and alkaline etching to form an intimately contacted Gr@eNi(OH) 2 -NiO composite. On one hand, Gr enables the highly dispersed distribution of Ni(OH) 2 /NiO species and improves the accessibility of active sites for the OER. On the other hand, Gr provides good electrical conductivity and rapid charge-transfer kinetic, leading to high catalytic activity. In 1 M KOH, Gr@eNi(OH) 2 -NiO delivers an overpotential of 260 mV at 10 mA cm −2 and Tafel slope of 41 mV dec −1 , together with stable operation in alkaline electrolyte. Macroscopic kinetics analysis based on current-overpotential fitting further suggests an enhanced potential response of the *OOH-forming step, consistent with improved OER kinetics enabled by Gr-deposit coupling. This work provides a practical route to integrate Ni hydroxide/oxide phases with Gr scaffolds for efficient alkaline water oxidation. Download: Download high-res image (334KB) Download: Download full-size image
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 12
·3568-3578
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IF 5
Menghui Liu,Chenhui Wang,Zifan Cao,Aiqun Kong,Yusheng Gao,Jinli Zhang,You Han,Wei Li,Yan Fu
A series of 3D self-standing PtRu/Ni(OH)2/NF electrodes is fabricated for electrocatalytic hydrogenation (ECH) of benzoic acid (BA) to cyclohexanecarboxylic acid (CCA). The PtRu/Ni(OH)2 electrocatalyst with a unique coral-shaped architecture possesses outstanding charge transfer ability and abundant active sites. The optimized electrode achieves a BA conversion of 99.00% and a CCA selectivity of 100% in 0.05 M H2SO4 within 80 min, showing a record faradaic efficiency of 43.90% and high performance during 20 cycles of ECH. In situ Raman tests verify the mechanism of the selective hydrogenation of the aromatic ring and density functional theory (DFT) calculations reveal that the electronic interaction between Pt and Ru in the PtRu nanoalloy as well as the electron transfer from the PtRu alloy to the Ni(OH)2 nanosheet tunes the electronic states of PtRu/Ni(OH)2, thereby enhancing the adsorption strength of BA on the electrocatalyst surface. This work offers a promising alternative to the traditional catalytic hydrogenation of BA.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 15
·7305-7311
·
IF 3.3
Jie Liu,Yu Chen,Yin Wang,Lu Liu,Qi Chen,Qingqing Shi,Luyi Huang,Xing Chen,Kun Xie
Cobalt phosphide has excellent electrical conductivity, metallic properties, and thermal stability. However, its application is limited due to the few active sites exposed in electrochemical reactions and poor structural stability. Herein, we adopt the strategies of material compounding and structural design to construct CoP@Ni(OH)2 bilayer nanosheets. The bilayer nanosheet structure can provide abundant transport paths for electrons and ions while also exposing more electroactive sites. In addition, the close contact and mutual support of the bilayer nanosheet structure can significantly alleviate material morphological collapse during charging/discharging processes, improving the cycle stability. The advantages of multiple components were combined in CoP@Ni(OH)2 to provide multiple valances for the faradaic redox reactions. The CoP@Ni(OH)2 manifested a specific capacity of 1697.8 C g−1 at 1 A g−1 and maintained a high rate capability of 35.0% even at 20 A g−1. Moreover, the electrode, had great cycling stability, retaining 83.9% of its capacity at 6 A g−1 after 7000 cycles. The asymmetric supercapacitor made of CoP@Ni(OH)2//activated carbon delivered 53.2 W h kg−1 at 800 W kg−1.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Chengbo Wei,Chuan Liu,Linna Gao,Yanfang Sun,Qingyun Liu,Xiao Zhang,Jinxue Guo
Integrating heterogeneous hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) electrocatalysts into compatible composite catalysts with specific interfaces and structures holds great promise for the development of efficient bifunctional catalysts for overall water splitting. Herein, heterogeneous MoS 2 -Ni(OH) 2 catalyst supported by Ni foam (MoS 2 @Ni(OH) 2 /NF) is developed, in which the Ni(OH) 2 nanorod array is grafted with MoS 2 nanosheets . The hierarchical 1D/2D structures benefit not only the exposure of catalytic site but also the facilitated charge transfer. The heterointerfaces allow the synergism of electric structure modulation for improved catalytic activity and kinetics towards HER, OER, and overall water splitting. MoS 2 @Ni(OH) 2 /NF achieves a current density of 10 mA cm −2 at low overpotentials of 134 and 233 mV for HER and OER in 1 M KOH, respectively. Moreover, a cell voltage as low as 1.46 V is obtained to afford 10 mA cm −2 in a tow-electrode electrolyzer using MoS 2 @Ni(OH) 2 /NF as bifunctional catalysts, assuring it superior to most of the reported noble-metal-free bifunctional electrocatalysts. Such heterogeneous design of composite catalyst should shed light on the exploration of functional materials for energy applications.
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CRYSTENGCOMM
·
2017
·Vol. 19
·期 38
·5780-5786
·
IF 3.474
Kun Ding,Xiao Zhang,Juping Li,Ping Yang,Xin Cheng
Ultrathin α-Co(OH)2 nanosheets (NSs) were hydrothermally synthesized without using surfactants and templates. Interestingly, the ultrathin α-Co(OH)2 NSs evolved from graphene-like NSs to hexagonal nanoplates (NPs) and then transformed into a needle-like Co(CO3)0.5(OH)·0.11H2O phase with increasing reaction temperature and time. The phase and morphology evolution depended strongly on the CO32− ions in the solution. We ruled out the possibility that CO32− originated from the adsorption of CO2 in air and proposed the possible phase transition mechanism from α-Co(OH)2 to Co(CO3)0.5(OH)·0.11H2O, which was due to the decomposition of hexamethylenetetramine driven by dynamics and thermodynamics. The morphology evolution could be regarded as the dissolution–recrystallization–redissolution–recrystallization of α-Co(OH)2. The electrochemical behavior tests demonstrated that the ultrathin α-Co(OH)2 electrode exhibited an excellent specific capacitance of 833.4 F g−1 at 5 A g−1; however, the specific capacitance of the needle-like Co(CO3)0.5(OH)·0.11H2O electrode was 247.2 F g−1 at the same current density. This excellent electrochemical property is attributed to the crystalline phase and ultrathin nature of the materials.
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ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Yan Gao,Lu Ye,Shuyan Cao,Hu Chen,Yanan Yao,Jian Jiang,Licheng Sun
Perovskite hydroxide CoSn(OH)6 nanoparticles were synthesized and used for the first time in the photocatalytic reduction of CO2 to CO. Under mild reaction conditions and using [Ru(bpy)3](PF6)2 as the photosensitizer, a high photocatalytic efficiency of 19.3 μmol for CO evolution with a high selectivity of 86.46% was obtained. The photocatalytic activity and CO selectivity were further improved by adding weak Brönsted acids, as proton sources, to the system.
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