Catalysts
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2021
·Vol. 11
·期 5
·561
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IF 4.146
Fangyuan Wang,Yu Liu,Zhiling Song,Zhichao Miao,Jinping Zhao
Electrochemical CO2reduction reaction (CO2RR) is eliciting considerable attention in relation to the carbon cycle and carbon neutrality. As for the practical application of CO2RR, the electrocatalyst is a crucial factor, but, even so, designing and synthesizing an excellent catalyst remains a significant challenge. In this paper, the coordination compound of Ni ions and dimethylglyoxime (DMG) was employed as a precursor to modify reduced graphene oxide (rGO) for CO2RR. The textural properties and chemical bonds of as-obtained rGO, N–C–rGO, Ni–rGO, Ni–N–C, and Ni–N–C–rGO materials were investigated in detail, and the role of Ni, N–C, and rGO in the CO2RR were researched and confirmed. Among all the catalysts, the Ni–N–C–rGO showed the optimal catalytic activity and selectivity with a high current density of 10 mA cm−2and FE(CO)% of 85% at −0.87 V vs. RHE. In addition, there was no obvious decrease in activity for 10 h. Therefore, the Ni–N–C–rGO is a promising catalyst for CO2RR to CO.Keywords:metallic Ni;N-doped carbon;reduced graphene oxide;electrocatalyst;electrochemical CO2reduction
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APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Xiaohan Yang,Hanbin Liu,Liwei Qian,Qingjun Meng,Haiwei Wu,Zhijian Li,Hongwei Zhou
The remediation of water that polluted by organic dyes and nanoparticles (NPs) remains a great challenge. However, second pollution of solid waste may produce if the adsorbents are not degradable or recyclable. The stimuli-responsive materials were regarded to be able to resolve this problem by reversible adsorption-desorption under stimuli. Here in this work, the surface of cellulose fibers was modified with CO 2 -responsive molecules through a simple esterification followed by an aza-Michael addition reaction. The chemical structure was confirmed with Fourier transform infrared spectra (FT-IR), X-ray photoelectron spectroscopy (XPS), x-ray diffractometer (XRD) and thermal analysis. The gas-responsiveness was demonstrated by monitoring of the pH, conductivity and surface zeta potential. Anionic dyes and negative charged NPs in water can be selectively and reversibly captured by the CO 2 -responsive surface on cellulose fibers, suggesting the inexpensive, readily available and smart cellulose fibers may find great potential in water remediation.
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JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING
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2021
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IF 4.346
Qi Wu,Yan Xu
Stimulus-responsive surfactant is becoming a hot research topic with high controllability and excellent emulsifying properties. In this work, an amidine naphthenate surfactant was synthesized for the first time by the reaction between alkyl amidine and naphthenic acid. Surface activity and emulsion performance of this novel surfactant in oil/water emulsion were investigated. Compared with the previously synthesized amidine bicarbonate surfactants, amidine naphthenate surfactants exhibited a superior emulsification performance above 60 °C due to their lower critical micelle concentration (CMC) and interfacial tension (IFT). The presence of two long alkyl groups is recognized as the main reason for its superior properties than amidine bicarbonate having only one long alkyl group. Increased hydrophobic interactions between the long alkyl chains and electrostatic interactions between the ionic head groups lead to the easier formation of micelles. Notably, the amidine naphthenate has a characteristic of CO 2 -responsive property. The amidine naphthenate emulsion can be demulsified by CO 2 bubbling which destroys the chemical structure of amidine naphthenate, accompanied by the formation of amidine cations and naphthenic acids. Then, the emulsion was completely demulsified due to the demulsification effect of naphthenic acid. Therefore, the synthesized amidine naphthenate surfactant possesses not only high interface activity but also CO 2 responsive property, which endows it an extensive application prospect for enhanced oil recovery (EOR) operations in the oil industry.
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Greenhouse Gases-Science and Technology
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2021
·Vol. 11
·期 6
·1191-1197
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IF 2.013
Subrato Acharjya,Jiacheng Chen,Minghui Zhu,Chong Peng
Immobilized tin phthalocyanine dichloride (SnPcCl 2 ) was prepared by refluxing SnPcCl 2 and hydroxyl-functionalized carbon nanotubes in DMF with the addition of triethylamine, which exhibited minimal aggregation and approximately 2–3 folds improvement in activity towards CO 2 electroreduction compared to the physically mixed SnPcCl 2 /CNT hybrid. Cyclic voltammetry analysis and in situ UV-vis spectra revealed that metallic tin is the active site for CO 2 electroreduction, and the redox behavior of Sn 0 is affected by the adjacent demetallized macrocycles. © 2021 Society of Chemical Industry and John Wiley & Sons, Ltd.
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ADVANCED FUNCTIONAL MATERIALS
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2021
·Vol. 31
·期 27
·2101255
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IF 18.808
Henglei Jia,Yuanyuan Yang,Tsz Him Chow,Han Zhang,Xiyue Liu,Jianfang Wang,Chun-yang Zhang
Symmetry-breaking synthesis of colloidal nanocrystals with desired structures and properties has aroused widespread interest in various fields, but the lack of robust synthetic protocols and the complex growth kinetics limit their practical applications. Herein, a general strategy is developed to synthesize the Au–Cu Janus nanocrystals (JNCs) through the site-selective growth of Cu nanodomains on Au nanocrystals, which is directed by the substantial lattice mismatch between them, with the assistance of judicious manipulation of the growth kinetics. This strategy can work on Au nanocrystals with different architectures for the achievement of diverse asymmetric Au–Cu hybrid nanostructures. Of particular note, the obtained Au nanobipyramids (Au NBPs)-based JNCs facilitate the conversion of CO 2 to C 2 hydrocarbon production during electrocatalysis, with the Faradaic efficiency and maximum partial current density being 4.1-fold and 6.4-fold higher than those of their monometallic Cu counterparts, respectively. The excellent electrocatalytic performances benefit from the special design of the Au–Cu Janus architectures and their tandem catalysis mechanism as well as the high-index facets on Au nanocrystals. This research provides a new approach to synthesize various hybrid Janus nanostructures, facilitating the study of structure-function relationship in the catalytic process and the rational design of efficient heterogeneous electrocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Shuaiqi Gong,Xue Teng,Yanli Niu,Xuan Liu,Mingze Xu,Chen Xu,Lvlv Ji,Zuofeng Chen
Zero-dimensional quantum dots (QDs) and two-dimensional nanosheets represent two kinds of distinctive materials with unique properties. Here, we describe the fabrication of step-scheme ( i.e. S-scheme) 0D/2D heterostructure with InVO 4 QDs and g -C 3 N 4 (CN) ultrathin nanosheets for photocatalytic CO 2 reduction. The formation of S-scheme heterostructure facilitates the separation of electron-hole pairs and reduces the recombination of charge carriers. Moreover, the light-absorption edge of InVO 4 /CN is extended to 605 nm because of the strong visible light absorption of InVO 4 QDs. The 0D/2D hybrid enables highly selective photocatalytic reduction of CO 2 to CO (93.3 %) at a decent rate of 69.8 μmol g −1 h −1 under visible light irradiation. Density functional theory (DFT) results suggest that the formation of InVO 4 /CN heterostructure can enhance CO 2 adsorption/activation, stabilize COOH* intermediates and allow rapid CO desorption as the major product. This study opens up a new possibility for construction of novel S-scheme heterostructure for photocatalytic applications.
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JOURNAL OF SUPERCRITICAL FLUIDS
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2021
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IF 4.577
Jian-Lei Qi,Qin-Qin Xu,Dan Zhou,Jian-Zhong Yin,Qi-Ke Jiang
Cu single atoms dispersed on N-doped carbon materials (Cu-NC) were obtained after supercritical CO 2 deposition and decompression, without further post-treatment. AC-HAADF-STEM, STEM , XRD , ICP-OES, and XPS results confirmed that the Cu atoms were equably dispersed over the N-doped carbon (NC) support with the loading of 0.80 wt%. The catalytic performance of Cu-NC in solvent-free oxidation of phenylcarbinol to benzaldehyde was investigated, and the conversion of 73.9% and selectivity of 85.7% were obtained at 50 °C for 1 h. A high-pressure view cell was used to observe the dissolution and diffusion for Cu(acac) 2 in scCO 2 . The stability of Cu-NC structures and the formation path of active oxygen species (O*) on different configurations were predicted by density functional theory (DFT) calculations, and CuN 3 C 1 was found to be more conducive to the activation of tert-butyl hydroperoxide (TBHP).
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ENERGY & FUELS
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2020
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IF 3.421
Houxiao Wu,Yinuo Yuan,Yongwei Chen,Daofei Lv,Shi Tu,Ying Wu,Zhong Li,Qibin Xia
CO2 capture and storage technologies have been adopted to eliminate anthropogenic CO2 emission. Compared with other methods, adsorptive separation technology using excellent adsorbents has attracted extensive attention for its operational flexibility and energy-efficient characteristics. Herein, we present a copper-based metal–organic framework, MOF-11, exhibiting highly efficient CO2/N2 (15:85, v/v) separation performance. There are two kinds of channels with different pore chemistries in the framework, in which dense Cu open metal sites (OMS) were found in channel I, while channel II had a narrower pore window size and was mainly decorated with −CH2 moieties from the organic ligands. At 298 K, the CO2 uptake value of MOF-11 was 4.63 mmol/g at 100 kPa and 2.92 mmol/g at 15 kPa, respectively, which was superior to many other reported MOF adsorbents. Molecular simulation indicated that CO2 dominantly occupied channel I due to the strong electrostatic interactions with the dense Cu OMS in channel I. In comparison, more N2 molecules were adsorbed into channel II through multiple weak van der Waals interactions with −CH2 moieties. Such a pore system gives MOF-11 high CO2/N2 selectivity (ca. 116 at 298 K). Moreover, the dynamic separation of CO2/N2 mixture gases on MOF-11 was further investigated by cyclic breakthrough experiments.
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APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Xiaoxue Zhao,Jingru Guan,Jinze Li,Xin Li,Huiqin Wang,Pengwei Huo,Yongsheng Yan
The conversion of CO 2 into high value-added carbon-based compounds through photocatalytic reduction technology is considered as one of the more promising strategies to solve the greenhouse effect. And construction of heterojunction photocatalysts can promote the separation of photoelectron-hole pairs, so as to achieve higher activity of photocatalytic CO 2 reduction. Hence, Pt@CeO 2 /3DCN heterojunction are prepared by calcination method and photoreduction technology. The photocatalytic results revealed that Pt@CeO 2 /3DCN show better photocatalytic activity for reducing CO 2 into CO and CH 4 , compared with 3DCN. Especially, Pt@45CeO 2 /3DCN shows the maximum photocatalytic activity of 4.69 and 3.03 μmol·h −1 ·g −1 for CO and CH 4 under UV light irradiation, respectively, and the reduction activity did not decrease significantly after five cycles. The enhanced photoreduction of CO 2 performance can be ascribed to the synergistic effects of the oxygen vacancies in CeO 2 for CO 2 activation and heterojunction for electron separation. Besides, Pt nanoparticles (NPs) on CeO 2 /3DCN can further promote the transfer of electrons, resulting in higher photocatalytic activity.
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CATALYSIS COMMUNICATIONS
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2020
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IF 3.612
Pengbo Wang,Qian He,Hao Zhang,Qingdi Sun,Yujie Cheng,Tao Gan,Xiaohui He,Hongbing Ji
Several research studies have been conducted on N -formylation of amines using phenylsilane and CO 2 . However, most of these studies involved tedious processes of catalyst preparation or complex procedures. In the present study, we describe the use of a simple and commercially available ZnO catalyst for selective N -formylation of amines under mild condition. High-yielding N -formylation products with good recyclability and wide substrate scope were obtained, which can promote fine chemical synthesis and CO 2 capture.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Bin Han,Xinwen Ou,Zuqi Zhong,Shujie Liang,Xu Yan,Hong Deng,Zhang Lin
Industrial wastes such as electroplating sludges and anthropogenic CO 2 , are misplaced resources whose utilization is severely hampered by their complex compositions or low concentration. Herein, on the basis of the specific binding characteristic of metal ions with small molecules, we demonstrate gradient-upcycling of solid wastes into different metal-organic frameworks (MOFs) for anthropogenic CO 2 -to-syngas photoconversion. In low-concentration CO 2 (10%), the as-prepared Ni MOFs exhibits record-high performance for CO 2 -to-CO photoconversion, while Fe MOFs favors for H 2 production. By taking Fe/Ni MOFs as the modular catalysts and adjusting their ratio, syngas with a widely tunable CO/H 2 ratio (1:15-14:1) was produced from CO 2 photoreduction. The diverse catalytic performance of Fe/Ni MOFs originates from the different affinities towards CO 2 /H 2 O, which relates to the 3d electron numbers of metal ions. We further confirm the universality of the gradient recovery approach to upcycle metal resources from solid wastes and the modular catalysts design approach for CO 2 -to-syngas photoconversion.
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GREEN CHEMISTRY
·
2020
·Vol. 22
·期 21
·7529-7536
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IF 9.48
Huihuang Chen,Xu Guo,Xiangdong Kong,Yulin Xing,Yan Liu,Bolong Yu,Qun-Xiang Li,Zhigang Geng,Rui Si,Jie Zeng
CO2 electroreduction into valuable products holds great promise for energy supply and environmental remediation but remains a challenge due to the lack of high-performance electrocatalysts. Herein, we developed an efficient strategy to prepare highly active Fe single-atom catalysts (Fe–N5/Fe–N6) by tuning the coordination number of Fe with N towards CO2 electroreduction. The faradaic efficiency of CO for Fe–N5 exceeded 90% ranging from −0.35 to −0.65 V versus the reversible hydrogen electrode (vs. RHE) towards CO2 electroreduction. The turnover frequency of CO for Fe–N5 reached 5006 h−1 at −1.05 V vs. RHE, which was 3.8 times that (1324 h−1) of Fe–N6. Besides, CO was generated at an overpotential as low as 50 mV over Fe–N5, smaller than that (90 mV) over Fe–N6. Density functional theory calculations demonstrated that Fe–N5 facilitated the adsorption and activation of CO2 to form the *COOH intermediate, thus leading to superior selectivity and activity for CO2 electroreduction.
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