CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Manlu Cheng,Xingyu Long,Ping Song,Zenghui Diao,Gang Song,Diyun Chen,Lingjun Kong
Stabilization of Co was essential to address its pollution. In this work, geopolymerization was used to stabilize the Co 2+ in the presence of alumina-silicate under hydrothermal process, in which the Co 2+ is hypothesized to be a substitute of cation to balance the charge. Then the Co 2+ could be incorporated into the geopolymer stably being named as Al x Si y Co z -T. Interestingly, the Co 2+ stabilized Al x Si y Co z -T was recycled and reused for peroxymonosulfate (PMS) activation. The stability and catalytic activity of the Al x Si y Co z -T in PMS activation was evaluated. Results showed that the alumina and silicate geopolymerization played positive role in Co 2+ stabilization, what were determined by the molar ratio of alumina to silicate, hydrothermal process. Besides, the Al x Si y Co z -T performed favorable activity in PMS activation for LEV degradation with an efficiency of 98.84 % and rate constant of 0.1154 min −1 . In this case, the Co 2+ was the main catalyst in PMS activation, while the alumina-silicate geopolymerization not only contributed to Co 2+ stabilization, but also resulted in the formation of oxygen vacancy. Then the co-catalytic of alumina-silicate in PMS activation was understood by the synergy factor. The Co 2+ leaching efficiency of AlSi 2 Co 4 -200 is only 0.011 %, confirming the heterogeneous catalytic in PMS activation. The Al x Si y Co z -200 performed favorable stability that could be used for five cycles at least. 1 O 2 , SO 4 − • and •OH contributed to LEV degradation. Thus, the alumina and silicate geopolymerization could play important role in stabilization and co-catalytic for activating PMS, performing the dual effect on waste treatment and resource recycle.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Haonan Yu,Xiaofeng Yang,Hongbin Yang,Jinming Xu,Yanqiang Huang
A phosphorus and nitrogen co-doped graphene (PNG) was developed via a two-step pyrolysis approach through the intermedium of g-C 3 N 4 template and glyphosate as the phosphorus source, and was used for the catalytic dehydrochlorination of 1,2-dichloroethane (EDC) to vinyl chloride monomer (VCM) production. The characterization results indicate that a volcano relationship of surface area and surface properties with the usage of phosphorus precursor was observed, and the sample of PNG-900-6 possesses not only the thin film structure with enhanced surface area but also the smaller grain size of PNG attachments. Accordingly, such PNGs show a great improvement of catalytic performance in the dehydrochlorination of EDC, and the PNG-900-6 catalyst behaves the best with a 4-times higher activity than that on the nitrogen doped graphene (NG). It was also proved that the synergetic effect of the unique P-C coordination on the graphene to generate more quaternary nitrogen species was crucial in determining the catalytic performance of EDC conversion. Our results demonstrate that the phosphorus and nitrogen co-doped graphene offers many advantages in physical structure and chemical property, and are also great potential on the catalytic application in the dehydrochlorination of 1,2-dichloroethane.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2023
·Vol. 27
·期 12
·3487-3504
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IF 2.5
Liu Cansen,Wu Xianhong,Xu Jianyu,Li Jinyan,Xie Huisi
Developing a coated metal mold to avoid scuff, corrosion, and fouling in rubber vulcanization condition remains challenging. Here, a composite coating is described which combines resistance to fouling, wear, and corrosion by incorporating low surface energy tungsten disulfide (WS 2 ) into a robust cobalt (Co) matrix for wear and corrosion resistance together with antifouling. The dispersity of WS 2 in the electroplating solution is improved by combining chemical modification with mechanical milling. The addition of 2 g/L WS 2 to the electroplating bath produced a Co-WS 2 composite coating with effective tribological and anticorrosion performance in 3.5 wt.% standing NaCl solution at 25 ℃ as well as superior antifouling behavior in rubber vulcanization conducted at 160 ℃ and 9.8 Mpa. Graphical Abstract
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npj Clean Water
·
2023
·Vol. 6
·期 1
·1-11
·
IF 11.4
Li Chao,Li Jiale,Huang Niu,Kong Xin Ying,Xiao Qingyi,Huang Yingping,Wong Po Keung,Ye Liqun
Advanced oxidation technology based on peroxonosulfate (PMS) has attracted extensive attention in water treatment research due to its fast reaction speed and wide pH range adaptability. Cobalt-based catalysts are considered to be one of the most effective reagents for PMS activation in various PMS activation methods. However, Co-ion leaching and difficulty in recovery have greatly hindered its practical applications. Herein, we developed a robust membrane constructed by nitrogen-doped carbon nanotubes embedded with cobalt nanoparticles (Co-NC) to concurrently address the Co-ion leaching and recovery issues. Based on our customization, continuous water flow reactor, the Co-NC membrane exhibited excellent catalytic activity and stability, in which it demonstrated a remarkable sterilization efficiency of 99.9999% against E. coli , and it retained a superior stability of 96.29% after 40 repeated cycles. Fewer attempts to put such efficient heterogeneous advanced oxidation processes (AOPs) into practical application, to mimic real-life applications, the performance of the Co-NC/PMS system was extended to the water taken from Qiuxi River. Remarkably, there is no deterioration in performance over 12 h of continuous real sewage processing. Mechanistic studies revealed that abundant high-valence metals (Co IV =O) were generated in the system, which can attack and penetrate into the cell membrane to destroy its intracellular defense system. This work provides useful insights into designing robust membranes with superior efficiency and stability for PMS-based advanced oxidation technology.
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BIOMACROMOLECULES
·
2023
·
IF 6.2
Chongkai Ji,Lijie Li,Yulin Nie,Rang Ping,Jiong Peng,Fuhang Song,Xin Li
The application of conductive hydrogels in flexible electronics has attracted much interest in recent years due to their excellent mechanical properties and conductivity. However, the development of conductive hydrogels combining with superior self-adhesion, mechanical properties, antifreeze, and antibacterial activity is still a challenge. Herein, inspired by the structure of the ligament, a multifunctional conductive hydrogel is constructed to address the issue by introducing collagen into the polyacrylamide. The obtained conductive hydrogel exhibits outstanding conductivity (52.08 mS/cm), ultra-stretchability (>2000%), self-adhesion, and antibacterial properties. More significantly, the supercapacitor based on this hydrogel electrolyte achieves a desirable capacitance (514.7 mF·cm–2 at 0.25 mA·cm–2 current density). As a wearable strain sensor, the obtained hydrogel can rapidly detect different movements of the body such as finger, wrist, elbow, and knee joints. It is conceived that this study would provide a potential approach for the preparation of conductive hydrogels in the application of flexible electronics.
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PubMed
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ENERGY CONVERSION AND MANAGEMENT
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2023
·
IF 10.4
Huping Yan,Zhen Liu,Ronghui Qi
Utilizing ambient humidity to drive electron motion in nanomaterials and generate usable electricity is promising for self-powered electronics and sensors. This paper developed a humidity gradient-driven microgenerator (HGDM) by coating a cobalt hydrogel on part of the TiO 2 nanoparticle film and employing multi-walled carbon nanotubes as electrodes. The humidity gradient was established between the bottom hygroscopic hydrogel and the top electrode in contact with ambient air. Results demonstrated that the TiO 2 /Co hydrogel HGDMs can achieve an open-circuit voltage of 0.95 V at 20 °C and 50–80% relative humidity (RH). The single generator (size: 5 × 4 cm 2 ) exhibited a current output of approximately 0.1 mA, which remained stable for over 100 h with less than 1% decay. The increase in hydrogel films’ height first increased then decrease the performance, and the optimal value was provided. By alternately introducing 10% and 80% RH air humidity cycles, the generator responded rapidly with a wet/dry output ratio over 400, and the delay time maintained within 1.0 s after 1000 cycles. The output performance dropped severely when the air temperature was higher than 40 °C. In practical applications, a series of 5–7 micro-generators successfully delivered consistent power supply to LED lights and calculators for a duration exceeding one week, and the voltage output can be recovered to its initial value after less than 5 h of recharging. Mechanistic studies have revealed that the primary driving force for power generation is the humidity gradient rather than vapor evaporation. Because the diameter of the nanopores (around 200 nm) are much smaller than the Debye length of the double electric layer (960 nm), ion-selective permeability in TiO 2 nanochannels is also important which can prevent nearly 90% OH – from passing through the channels. This hydrogel microgenerator exhibits wide-ranging application prospects, and our study contributes to enhancing its performance and elucidating the mechanism.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Chengcheng Qi,Chongchao Zhang,Ziyin Yang
Defect engineering was considered as an effective strategy to regulate electrocatalytic activities of transition metal oxides . However, there are seldom reports about metal defects in electrochemical sensing. In this work, Co-defected Co 3 O 4 was synthesized via thermal treatment of glycerolatocobalt (CoGly) precursor for constructing a novel electrochemical nonenzymatic glucose sensor. The obtained nanomaterials were characterized by transmission electron microscopy (TEM), powder X-ray diffractometry (XRD), Raman spectra , X-ray photoelectron spectroscopy (XPS) and electrochemical techniques . The presence of Co defects regulated electronic structure of Co 3 O 4 , which not only speeds up electron transfer rate but also exposes more high-valent Co sites, thus improving electrocatalytic activities. Under optimized conditions, Co-defected Co 3 O 4 electrode exhibited excellent performance for glucose analysis with a wide linear range of 0.2 µM to 0.5 mM, a low detection limit of 0.16 µM. Importantly, an ultrahigh sensitivity of 2595.7 µA·mM −1 ·cm −2 was also obtained, which was about 10 times higher than that of conventional Co 3 O 4 . Therefore, engineering Co 3 O 4 with Co defects is an effective strategy to tailor electrocatalytic activity, which sheds light on the potential applications of metal defects in the field of electrochemical nonenzymatic sensing.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 44
·17081-17088
·
IF 4.569
Wenyuan Wang,Kai Zhang,Tao Xu,Yagang Yao
Nowadays, the goal of carbon peaking and carbon neutrality has become a global consensus, and electrochemical CO2 reduction to provide high-value power fuel is one of the major technical approaches attracting significant research interests and application prospects. However, the inevitable hydrogen evolution reaction in water-based electrolyte systems crowds out the reactive sites of active metals, causing a low CO2 conversion efficiency. In this work, Zn nanosheets were prepared via electrodeposition on the surface of carbon paper and then modified with polytetrafluoroethylene (PTFE) to tune the wetting angle of the electrolyte. A CO faradaic efficiency of 90.2% was achieved for Zn NS-8% PTFE (contact angle: 136.8°) at the electrolytic voltage of −1.0 V vs. RHE along with an overall current density of −7.9 mA cm−2. Experimental results and molecular dynamics simulation revealed that PTFE weakened the aggregation of H2O molecules and was more beneficial for capturing and adsorbing CO2 molecules near the electrode surface. The active sites of hydrogen production were transformed into the reaction center for electrocatalytic CO2 reduction due to the hydrophobicity of the electrode, and the accumulation of the local CO2 concentration accelerated the kinetic activity for electrochemical conversion (CO2 to CO). This strategy of tuning the local environment offers an alternative approach for effective electrode manufacturing in liquid electrolytes.
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FUEL
·
2022
·
IF 8.035
Zeng Zhang,Fei Wang,Jianchun Jiang,Hao Zhu,Yuchan Du,Junfeng Feng,Hui Li,Xiaoxiang Jiang
Lipid hydrotreatment to generate green diesel can weaken the dependence on unrenewable fossil fuels. The catalytic performance of Co catalyst is greatly limited by the dispersion and the number of Co active sites. To solve this problem, the Co-Al nanosheet was synthesized by using Co-Al LDH as the precursor. In the fatty acid hydrotreatment at 220 °C, the Co-Al nanosheet attained 98.0 % conversion and 64.3 % alkane yield, much higher than that of the Co/Al 2 O 3 catalyst (83.7 % conversion and 18.7 % alkane yield). From the catalyst characterizations, the excellent activity of Co-Al nanosheet was mainly ascribed to its high Co content and lamellar structure, exposing massive Co sites with high dispersion and small particle size. In addition, the high percentage of weak acidity, strong interaction between support and Co sites, and the improvement of the decarboxylation route also contributed to its catalytic performance. Moreover, the kinetics of octadecanol hydrotreatment over Co-Al nanosheet and Co/Al 2 O 3 revealed that octadecanol hydrotreatment more easily occurred over Co-Al nanosheet regarding the lower activation energy.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
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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CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Reziwanguli Yantake,Palidan Aierken,Aierken Sidike
The cyan emission band contains blue and green light regions, which can simplify the fabrication process of white light-emitting diodes and help promote the development of solid-state lighting. In this paper, a series of Eu 2+ singly doped and Eu 2+ and Li + co-doped cyan light-emitting KAlSiO 4 : x Eu 2+ , y Li + materials were synthesized using the high temperature solid-state method. It was found that the incorporation of 10% Li + could increase the emission intensity of the KAlSiO 4 :0.02Eu 2+ sample by up to a factor of ∼3. This also shifted the emission color of the sample from blue-cyan (472 nm) to cyan (485 nm), and the quantum yield was increased from 71.5% to 93.3%. When the temperature is increased to 150 °C, the peak emission intensity was increased from 75.9% to 92.7% of that at room temperature. DFT calculations were used to demonstrate that the KAlSiO 4 phosphor host possesses a wide bandgap of 4.86 eV and the experimentally-determined optical bandgap of the phosphor was 5.6 eV. The phosphor was combined with a commercial red phosphor, and these together were used as the emitting components in a white LED package. The characteristics of the white LED when using two representative samples of the phosphor (KAlSiO 4 : 0.02Eu 2+ and KAlSiO 4 : 0.02Eu 2+ , 0.1Li + ) were examined; these white LEDs had color rendering indices of 82 and 95, and color temperatures of 5656 K and 4126 K respectively. This work demonstrates the significant potential that KAlSiO 4 :0.02 Eu 2+ , 0.1 Li + phosphors have in the field of LED lighting.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 43
·20809-20816
·
IF 3.925
Ziying Li,Linlin Zang,Qing Xu,Fengtong Shen,Jingzhen Wang,Ying Zhang,Yanhong Zhang,Liguo Sun
The electrochemical hydrogen evolution reaction (HER) requires highly efficient electrocatalysts with durable and stable performance. In this work, multiwalled carbon nanotubes (MWCNTs) are employed as electrocatalyst carriers, polystyrene microspheres as templates, chitosan as a nitrogen-doped carbon (N–Carbon) source, and cobalt nitrate as a cobalt source to manufacture hollow Co nanoparticle and N–carbon modified CNT (Co/NCNT) composite foam as highly efficient electrocatalysts with durable and stable performance. This composite foam not only has a fast electron transfer rate but also contains more exposed intact sites and ion transport channels, making ion storage and movement easier. In addition, hollow Co nanoparticles (NPs) enhanced the catalyst activity and N–Carbon and MWCNTs enhanced the electrical conductivity of the carbon matrix. The coupling between the hollow Co NPs, N–Carbon, and MWCNTs enhances the electrocatalytic performance of the electrocatalyst in the HER. Compared with other electrocatalysts, the Co/NCNT exhibits lower overpotential (20 mV) at a current density of 10 mA cm−2, lower Tafel slope (27.53 mV dec−1) and stronger cycling durability (2000 cycles) in 1 M KOH. The composite foam developed here may be a potential high-performance HER catalyst.
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