TALANTA
·
2021
·
IF 6.057
Lijun Xu,Dongguo Xue,Jialin Sai,Lu Zhou,Renjun Pei,Aihua Liu
Although enzyme mimics have been widely developed, limited catalytic efficiency is still a bottleneck, especially under neutral condition. Herein, we reported the bioactive quinaldic acid (QA) significantly boosted the peroxidase-like activity of Co 2+ in the presence of bicarbonate (HCO 3 − ). With 2,2′-azino-bis-(3-ethylbenzothiazoline-6-sulphonate) (ABTS) as the substrate, the catalytic activity of Co 2+ (1 μM) was increased by over 300 times upon adding 100 μM QA. The formed Co 2+ complex had much higher turnover number (5.52 min −1 ) than that of cobalt-based nanozymes (0.011–0.51 min −1 ) in decomposing H 2 O 2 . Based on this system, ultrasensitive colorimetric methods for the detection of Co 2+ , bicarbonate and urease activity were achieved with limits of detection of 4.6 nM, 40 μM and 0.00125 U/mL, respectively. For the first time, this work established an ultrasensitive method for the detection of urease activity by activating a peroxidase-like mimic with the produced HCO 3 − .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 2
·823-835
·
IF 2.081
Wang Ying,He Runfa,Wang Cong,Li Gang
A kind of heterogeneous catalyst MCM-41-S-ImBr was prepared by grafting 1-vinyl-3-ethylimidazolium bromide ([VEIM]Br) on the surface of MCM-41. The catalyst was characterized by X-ray diffraction patterns, Fourier transform infrared spectroscopy and element analysis as well as scanning electron microscopy. It showed that [VEIM]Br was successfully grafted on MCM-41 and the catalyst possessed an average particle size of 1.4 µm with intact mesoporous structure. Moreover, the catalyst exhibited high catalytic activity in the cycloaddition reaction of CO 2 with epichlorohydrin without co-catalyst. The conversion of epichlorohydrin was 98.5% and the selectivity of cyclic carbonate was 98.3% at 130 °C under 1.6 MPa for 6 h. Reaction kinetic study indicated that the pseudo-first order rate constant was 0.223 ± 0.001 h −1 . It is proved that MCM-41-S-ImBr could be used at least 4 times without obvious decrease in catalytic performance. A possible reaction mechanism was also proposed: the quaternary imidazolium ion cooperatively worked with the bromide ion to catalyze the reaction. Graphical Abstract
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Feng Sha,Chizhou Tang,Shan Tang,Qingnan Wang,Zhe Han,Jijie Wang,Can Li
Catalytic conversion of CO 2 into methanol utilizing green hydrogen produced from renewable energy is a promising route to realize carbon neutrality. Although ZnZrO x solid solution catalyst displays excellent catalytic performance, it is still highly desired to make any further improvement. Herein, we found the promoting effect of incorporating Ga into ZnZrO x solid solution catalyst in CO 2 hydrogenation to methanol. Ga promoted ZnZrO x (GaZnZrO x ) solid solution catalyst exhibits CO 2 conversion of 8.8% and methanol space time yield of 630 mg g cat −1 h −1 that are higher than those of ZnZrO x solid solution catalyst (7.7%, 556 mg g cat −1 h −1 ) at 320 °C, while the highly selectivity toward methanol remains unchanged. Chemisorption and H 2 -D 2 exchange results show that GaZnZrO x solid solution catalyst displays higher capacity for the adsorption and activation of H 2 than ZnZrO x solid solution catalyst. Electron paramagnetic resonance result suggests that more oxygen vacancies are derived after incorporating Ga into ZnZrO x solid solution catalyst. In situ diffuse reflectance infrared Fourier transform spectra indicate that the HCOO* and CH 3 O* species are the main intermediate species. The higher IR intensity of intermediate species and lower CH 3 O*/HCOO* ratio on GaZnZrO x solid solution catalyst suggest that the hydrogenation of HCOO* to CH 3 O* is boosted. These results reveal the promoting effect of incorporated Ga into ZnZrO x solid solution catalyst that improves the adsorption and activation of H 2 and CO 2 , thus enhancing catalytic performance of methanol synthesis from CO 2 hydrogenation.
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2021
·
IF 4.837
Jianhua Ge,Bin Han,Shujie Liang,Zhongfei Liu,Yuhua Xiao,Juner Kuang,Minghui Guan,Xueming Liu
Direct photoconversion of diluted CO 2 into solar fuels has theoretically and practically become a hot research topic. However, the low yields and poor selectivity of carbonaceous products hampered by the H 2 evolution reaction is still a challenge for its practical application. Herein, we demonstrate a three-dimensional (3D) nickel borate/graphene nanoarrays (Ni-B i /G) for diluted CO 2 photoreduction with boosted activity and selectivity. In simulated flue gas with 10% CO 2 , the pristine Ni-B i displays a low activity and low CO selectivity of 41.8%, indicating its tendency of producing H 2 in diluted CO 2 . However, after growing Ni-B i nanoarrays onto graphene nanosheets , the optimized 3D Ni-B i /G exhibits a high CO selectivity of 84.9% with a CO production rate of 5.1 μmol h −1 , which is about 2 times of the blank sample. The improved performance can be attributed to the synergistic effect of the introduction of rGO and unique 3D structure, which are conducive not only to accelerate the separation of photogenerated charges, but also to enrich active sites and enhance CO 2 adsorption. This work provides fundamental guidance to the rational design of well-designed hierarchical catalysts for photoconversion of low concentration CO 2 .
✓ 已验证
产品关联
DOI
高影响因子
Processes
·
2021
·Vol. 9
·期 12
·2140
·
IF 2.847
Bin Liu,Zhe Cui,Wende Tian
Tertiary amines have been used as alternative absorbents for traditional primary and secondary amines in the process of carbon capture. However, the carbon dioxide (CO2) absorption rates in these kinds of amine are relatively slow, which implies greater investment and construction costs and limits the large-scale application of carbon capture. Carbonic anhydrase (CA) is considered to be an ideal homogeneous catalyst for accelerating the rate of CO2into aqueous amine solution. In this work, CO2absorption combining CA with two single aqueous tertiary amines, namely triethanolamine (TEA) and 2-(diethylamino)ethanol (DEEA), was studied by use of the stopped-flow apparatus over temperature ranging from 293 to 313 K. The concentrations of selected aqueous amine solution and CA used in the experiment were ranging among 0.1–0.5 kmol/m3and 0–50 g/m3, respectively. Compared to the solution without the addition of CA, the pseudo first-order reaction rate in the presence of CA (k0,withCA) is significantly increased. The values ofk0,withCAhave been calculated by a new kinetics model. The results of experimental and calculatedk0,amineandk0,withCAin CO2-amine-H2O solutions were also investigated, respectively.Keywords:carbon capture;CO2absorption;carbonic anhydrase;reaction kinetics
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Chuanhong Wang,Jun Zhang,Zhonggang Wang
Four nonfluorinated and fluorinated nanoporous polymers [PAN-5H, PAN-5F, PAN-2F, and PAN-2(CF3)] were synthesized from a triazine-based tetramine with benzaldehyde, pentafluorobenzaldehyde, 3,5-difluorobenzaldehyde, and 3,5-bis(trifluoromethyl)benzaldehyde, respectively. It is interestingly found that the porosity parameters and selective adsorptions of CO2 and light hydrocarbons strongly depend not only on the number and kind of fluorine atoms and fluorinated groups, but also on the substituted position on the phenyl rings in the fluorinated porous polymers. Relative to PAN-5H and PAN-5F, PAN-2F, and PAN-2(CF3) with phenyls meta-substituted by two fluorinated groups exhibit considerably increased BET surface areas from 502 to 1269 m2/g. At 298 K and 1 bar, the uptakes of C3H8, C2H6, and C2H4 in PAN-2F reach 4.62, 3.64, and 3.20 mmol/g, respectively, whereas PAN-5F exhibits the highest adsorption selectivities of C3H8/CH4 (372.3), C3H8/CO2 (33.2), C2H6/CH4 (21.8), C3H8/C2H6 (9.4), and CO2/CH4 (7.1) among the four polymers. The dynamic breakthrough experiments demonstrate that the mixed gases of C2H6/C2H4, C3H8/CH4, C2H6/CH4, and CO2/CH4 can be separated by the fluorinated polymers under ambient condition. The achieved results are significant for understanding the effects of fluorine-functionalization on the separation of ethylene and CO2 from light hydrocarbons in nanoporous polymers.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Jiehong He,Pin Lyu,Bo Jiang,Shaoshuai Chang,Haoran Du,Jian Zhu,Hexing Li
Photocatalytic CO 2 hydrogenation into fuels and value-added chemicals is considered as a promising strategy for CO 2 conversion and utilization. However, the photocatalysts used usually displays low efficiency and poor durability. Herein we developed a novel catalyst by combining NiB amorphous alloy with In 2 O 3 semiconductor, which exhibited very high HCOOH yield (5158.0 umol g −1 h −1 ) in CO 2 hydrogenation under sunlight irradiation. The In 2 O 3 acted as a photocatalyst for generating photoelectrons to reduce CO 2 and provided sufficient surface hydroxyl (In−OH) groups favouring CO 2 adsorption during the reaction. The high dispersion of NiB nanoparticles (co-catalyst) and interaction with In 2 O 3 provided the rich interface between NiB and In 2 O 3 , favoring the surface reactions between CO 2 and H 2 . Meanwhile, the unique amorphous alloy structure made the Ni electron-enriched, which promoted CO 2 hydrogenation through the H 2 dissociation. More importantly, the NiB amorphous alloy with good electric conductivity facilitated the transfer of photoelectrons from In 2 O 3 , which sufficiently diminished the photoelectron-hole recombination, leading to the enhanced quantum efficiency in photocatalytic CO 2 hydrogenation.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiao-Xue Wang,Gui-Juan Ji,Ping She,Fei Li,Qing-Chao Liu,Huan-Feng Wang,Ji-Jing Xu
The hysteresis kinetics of carbon dioxide reduction reaction (CDRR) and evolution reaction (CDER) reaction are major barriers toward the practical implementation of lithium-carbon dioxide (Li-CO 2 ) batteries. Herein, a free-standing and binder-free cathode composed of rutile TiO 2 nanorod arrays (TiO 2 NAs) and carbonized natural sponge was designed and realized by a simple seeds-assisted construction. The novel air cathode was found to exhibits a high specific capacity of 4.38 mAh cm −2 and long cycle life of more than 1600 h, as well as the discharge products, which would deposit at the surface of the TiO 2 NAs rather than carbon substrate during the discharge process. The improved performance can be ascribed to the interconnected conductive sponge framework with macropore and mesoporous channels that can house more discharge products, and the reactant molecules can unrestricted contact with the active sites. Furthermore, the good adhesion to the carbon substrate and the numerous available catalytic sites of the TiO 2 NAs contribute intimate contact of the discharge products with the TiO 2 NAs, improving CDRR and CDER kinetics effectively and boosting the electrochemical reactions. This TiO 2 /Sponge represents a promising design in the development of a nature-inspired, self-standing, and binder-free electrode for high-performance Li-CO 2 batteries.
✓ 已验证
产品关联
DOI
高影响因子
Nature Catalysis
·
2021
·Vol. 4
·期 3
·202-211
·
IF 41.813
Liu Hongfei,Xia Jun,Zhang Nan,Cheng Han,Bi Wentuan,Zu Xiaolong,Chu Wangsheng,Wu HengAn,Wu Changzheng,Xie Yi
Conventional strategies for modifying electrocatalysts for efficient CO 2 reduction are mainly based on doping, defect/morphology engineering, substrate design and so on. In most cases, these methods can only tune their structures, electronic states and thereby catalytic properties in a gradual way. Here we report that the solid–liquid phase transition of Ga–Sn/Ga–In alloys can induce an instant and radical transformation of their atomic and electronic structures during electrocatalysis, which dramatically impacts their catalytic properties. The transition of Sn/In active components from phase-segregated clusters to dispersed single atoms during melting results in a unique electronic structure through further reduction of both metallic Sn/In and Ga. Such atomic/electronic structure transitions can correlate well with suppression of the hydrogen evolution reaction and an enhanced formate Faradaic efficiency from <35% to >95%. This two-state switching strategy may be extended to other catalytic reactions to determine correlations between their structures and catalytic properties.
✓ 已验证
产品关联
DOI
高影响因子
Materials Science & Engineering C-Materials for Biological Applications
·
2021
·
IF 7.328
Xiangping Wen,Guangming Wen,Wenyan Li,Zhonghua Zhao,Xine Duan,Wenjun Yan,John F. Trant,Yingqi Li
Fluorescent carbon dots (CDs) were hydrothermally synthesized from a mixture of frozen tofu, ethylenediamine and phosphoric acid in an efficient 64% yield. The resulting CDs exhibit good water solubility, low cytotoxicity, high stability, and excellent biocompatibility. The CDs selectively and sensitively detect Co 2+ through fluorescent quenching with a detection limit of 58 nM. Fluorescence can be restored through the introduction of EDTA, and this phenomenon can be used to quantify EDTA in solution with a detection limit of 98 nM. As both analytes are detected by the same CD platform, this is an “off-on” fluorescence sensor for Co 2+ and EDTA. The technique's robustness for real-world samples was illustrated by quantifying cobalt in tap water and EDTA in contact lens solution. The CDs were also evaluated for in vivo imaging as they show low cytotoxicity and excellent cellular uptake. In a zebrafish model, the CDs are rapidly adsorbed from the intestine into the liver, and are essentially cleared from the body in 24 h with no appreciable bioaccumulation. Their simple and efficient synthesis, combined with excellent physical and chemical performance, renders these CDs attractive candidates for theranostic applications in targeted “smart” drug delivery and bioimaging.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanomaterials
·
2021
·Vol. 11
·期 3
·694
·
IF 5.076
Ruoxin Yuan,Hao Wen,Li Zeng,Xi Li,Xingang Liu,Chuhong Zhang
Supercritical CO2(scCO2) is often used to prepare graphene/metal oxide nanocomposite anodes for high performance lithium-ion batteries (LIBs) by the assisted solvothermal method due to its low viscosity, high diffusion, zero surface tension and good surface wettability. However, the formation mechanism of metal oxides and the combination mechanism between metal oxides and graphene in this system are superficial. In this work, a cobalt monoxide/graphene (CoO/G) nanocomposite is fabricated via the scCO2assisted solvothermal method followed by thermal treatment. We elucidate the mechanism that amorphous intermediates obtain by the scCO2assisted solvothermal method, and then ultrafine CoO nanoparticles are crystallized during the heat treatment. In addition, scCO2can promote CoO to be tightly fixed on the surface of graphene nanosheets by interfacial chemical bonds, which can effectively improve its cycle stability and rate performance. As expected, the CoO/G composites exhibit higher specific capacity (961 mAh g−1at 100 mA g−1), excellent cyclic stability and rate capability (617 mAh g−1after 500 cycles at 1000 mA g−1) when applied as an anode of LIB.Keywords:lithium-ion battery;anode;supercritical carbon dioxide;cobalt monoxide;graphene
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
·
2021
·
IF 2.262
Shanshan Dai,Minmin Tao,Hongsheng Lu
CO2-responsive wormlike micelles based on ionic liquid 1,1,3,3-tetramethylguanidine-oleic acid (TMG-OA) and cationic surfactant tetradecyl trimethyl ammonium bromide (TTAB) was designed in this work, avoiding the volatileness and flammability of traditional wormlike micelles formed with amines. It provides a new method of preparing CO2-switchable wormlike micelles based on ionic liquid with acidic group. The ionic liquid TMG-OA was prepared by the direct neutralization reaction between TMG and HOA at the molar ratio of 1:1. Due to the excellent stability and switchability demonstrated by thermogravimetry (TGA) and pH, TMG-OA can be treated as nonvolatile surfactant with CO2-responsive acidic group. Then the worm-based viscoelastic fluid is formed by the electrostatic interaction between TTAB and TMG-OA, and the steady and dynamic rheology show that the viscoelastic fluid has CO2-switchable thinning behavior. The switchable behavior is consistent with the reversible transition of microstructure from wormlike micelles to emulsion, which were detected by the dynamic light scattering (DLS) and cryo-transmission electron microscope (Cryo-TEM). The microstructural transition is induced by the reversible conversation between TMG-OA component and HOA component upon CO2 and N2/heat.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）