ChemSusChem
·
2019
·Vol. 12
·期 12
·2740-2747
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IF 7.804
Xiaoli Jin,Chade Lv,Xin Zhou,Liqun Ye,Haiquan Xie,Yue Liu,Huan Su,Biao Zhang,Gang Chen
Graphical Triple boost ! The high abundance of oxygen vacancies in Bi 24 O 31 Cl 10 play the following three roles for fully optimizing the CO 2 conversion efficiency: (i) enhance charge density, (ii) improve separation of electron–hole pairs, and (iii) lower energy for the formation of intermediates during the process. Unearthing an ideal model to describe the role of defect sites for boosting photocatalytic CO 2 reduction is rational and necessary, but it still remains a significant challenge. Herein, oxygen vacancies are introduced on the surface of Bi 24 O 31 Cl 10 photocatalyst (Bi 24 O 31 Cl 10 -OV) for fine-tuning the photocatalytic efficiency. The formation of oxygen vacancies leads to a new donor level near the conduction band minimum, which enables a faster charge transfer and higher carrier density. Moreover, oxygen vacancies can considerably reduce the energy for the formation of COOH* intermediates during CO 2 conversion. As a result, the activity of Bi 24 O 31 Cl 10 -OV for selective photoreduction of CO 2 to CO is significantly improved, with a CO generation rate of 0.9 μmol h −1 g −1 , which is nearly 4 times higher than that of pristine Bi 24 O 31 Cl 10 . This study reinforces our understanding of defect engineering in Bi-based photocatalysts and underscores the potential importance of implanting oxygen vacancies as an effective strategy for solar energy conversion.
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JOURNAL OF ELECTRONIC MATERIALS
·
2016
·Vol. 46
·期 2
·999-1004
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IF 1.491
Huang Zhengfeng,Cheng Xudong,Dong Peimei,Zhang Xiwen
To mitigate the greenhouse effect, many studies have been carried out to improve the CO 2 conversion efficiency of TiO 2 . Modification of TiO 2 has been intensively investigated, but the influence of an electric field on photoreduction by this material remains largely unknown. Accordingly, in this study, we explored the effect of an electric field on the photoreduction process using a porous TiO 2 -Ti material. The results indicated that the CO yield improved 85-fold (equivalent to 4772 μ mol/g h) when a 30-kV voltage was applied during the reduction process. To make the electric field effect fully functional, we also explored the effect of water on the photoreduction process, finding that TiO 2 showed the highest conversion rate when the humidity was controlled at 50% relative humidity (RH).
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CARBON
·
2019
·
IF 7.466
Yawei Yue,Yangye Sun,Can Tang,Bing Liu,Zhe Ji,Anqi Hu,Bin Shen,Zizhong Zhang,Zhengzong Sun
To reverse the ever-increasing trend of the CO 2 concentration in the atmosphere, human needs to develop a killer “catalyst”, which could convert the anthropogenic CO 2 back into high value-added or energy-storage molecules, not under the natural photosynthesis Calvin cycle, but through an artificial CO 2 reduction pathway. In the race to this emergent technology, the electrochemical reduction of CO 2 (CO 2 RR) with carbon based catalyst becomes one of the frontrunners. However, the carbon-based catalysts are genetically complex, with edge, strain, intrinsic topological defect, and doping effects, coexisting and affecting the catalysis behavior. Without a relative activity ranking system under the same metrics, unveiling the mechanism and improving the catalyst would become formidable. Here we assessed different carbon materials’ CO 2 RR performance under standard experimental conditions. The catalytic activities were evaluated and sequenced by their cathodic potential, characterized with the peak CO faradic efficiency . The doping effect is leading in the sequence, followed with the other three factors, all of which are superior to the pristine sp 2 carbon material.
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ACS Applied Nano Materials
·
2020
·
IF 0
Siyu Kuang,Minglu Li,Rong Xia,Lei Xing,Yaqiong Su,Qun Fan,Jinping Liu,Emiel J.M. Hensen,Xinbin Ma,Sheng Zhang
The electrochemical carbon dioxide reduction reaction (CO2RR) is a promising solution to the current environmental and energy issues. Cu is the only metal catalyst able to convert CO2 into high-value-added hydrocarbons. However, Cu catalysts tend to degrade with the decrease in the hydrocarbon selectivity under operation conditions. Herein, we monitored the morphological evolution of Cu nanocatalysts and correlated with changes in the selectivity of hydrocarbon products during electrochemical CO2 reduction. Initial Cu nanospheres quickly reconstructed into nanocubes within 1 h of CO2 electrolysis and then gradually turned into even smaller irregular nanoparticles. Interestingly, the above unstable Cu nanocube offered the maximum ethylene selectivity. We successfully stabilized these Cu nanocubes using a 2D graphene surface doped with nitrogen to achieve high ethylene selectivity over 24 h. Our X-ray photoelectron spectroscopy (XPS) and density-functional theory (DFT) investigations show that the strong interaction between Cu and pyridinic nitrogen on the 2D graphene surface plays a key role in stabilizing Cu nanocubes.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Haiyang Zhang,Ruili Guo,Jinli Zhang,Xueqin Li
Mixed matrix membranes (MMMs) have exhibited advantages in overcoming the trade-off effect, although it is still intensively demanded in the design of multifunctional fillers to improve CO2 separation performance. At present, MMMs with transport channels present an effective strategy to obtain ultrahigh CO2 permselectivity. In this work, Pebax-based MMMs was fabricated by incorporating nanocapsules (NCs), whose exterior, interior and transverse shell surfaces contained abundant carboxylic acid groups. NCs, similar to vesicles in cells, provide favorable physical and chemical microenvironments to the constructed CO2 transport channels, enhancing the CO2 permselectivity via both a facilitated transport mechanism and a solution-diffusion mechanism. CO2 permselectivity of MMMs doped with 20 wt % NCs surpassed the 2008 Robeson limit; an increase in CO2 permeability was up to 1431 ± 35 Barrer for pure gas, which was a 362% enhancement from the pure membrane, and an increase of the CO2/CH4 and CO2/N2 ideal selectivities to 46 ± 1.4 and 69 ± 2.7, corresponding to 44% and 23% enhancements from the pure membrane, respectively. This study provides an ingenious strategy to enhance the gas permselectivity of MMMs.
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NANO
·
2019
·
IF 1.293
Hongning Wang,Chao Xu,Yongsheng Zhou,Wenpu Zhao,Jing Zhong,Weiqiu Huang,Ruoyu Chen
Hierarchical N-doped carbon nanotubes (NCTs) with controllable aspect ratios were developed for CO 2 adsorption. In this work, NCTs were synthesized by coating different amounts of 3-aminophenol/formaldehyde resin (APF) on the outer layer of silica nanotubes, carbonizing in N 2 at 700 ∘ C and removing the silica and Ni template by hydrofluoric acid etching. The obtained NCTs were activated by K 2 CO 3 . After activation, micropores on the activated N-doped carbon nanotubes (ANCTs) were enriched, the micro-surface area and pore volume of ANCT-1.0 reached 1195 m 2 g − 1 and 0.45 cm 3 g − 1 , respectively, and the corresponding adsorption capacity increased by 50% (4.50 mmol g − 1 at 0 ∘ C and 1 bar). Moreover, ANCT-1.0 maintained a high stability throughout consecutive adsorption–desorption cycles. The advantages of hierarchical N-doped carbon nanotubes, including their meso–microporous structures, high geometric aspect ratio and good stability, make them valuable and promising materials to capture carbon dioxide.
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Science China-Chemistry
·
2019
·Vol. 62
·期 12
·1710-1719
·
IF 6.085
Wang Guishuo,Luo Ran,Yang Chengsheng,Song Jimin,Xiong Chuanye,Tian Hao,Zhao Zhi-Jian,Mu Rentao,Gong Jinlong
Metal oxide-promoted Rh-based catalysts have been widely used for CO 2 hydrogenation, especially for the ethanol synthesis. However, this reaction usually suffers low CO 2 conversion and alcohols selectivity due to the formation of byproducts methane and CO. This paper describes an efficient vanadium oxide promoted Rh-based catalysts confined in mesopore MCM-41. The Rh-0.3VO x /MCM-41 catalyst shows superior conversion (~12%) and ethanol selectivity (~24%) for CO 2 hydrogenation. The promoting effect can be attributed to the synergism of high Rh dispersion by the confinement effect of MCM-41 and the formation of VO x -Rh interface sites. Experimental and theoretical results indicate the formation of til-CO at VO x -Rh interface sites is easily dissociated into *CH x , and then *CH x can be inserted by CO to form CH 3 CO*, followed by CH 3 CO* hydrogenation to ethanol.
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JOURNAL OF ORGANIC CHEMISTRY
·
2023
·
IF 3.6
Yunying Yan,Jianjun Hao,Fenfen Xie,Fen Han,Linhai Jing,Pan Han
Magnesium-mediated reductive carboxylation of p-QMs with CO2 via an Umpolung strategy has been developed, which can be used for the preparation of various aryl acetic acids. This protocol featured high atom economy, mild conditions, and operational simplicity. The creation of this Umpolung carboxylation of p-QMs will unprecedentedly extend the application of p-QMs to nucleophilic reagents.
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LETTERS IN ORGANIC CHEMISTRY
·
2023
·Vol. 20
·期 4
·370-375
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IF 0.8
Chai Mengliang,Wu Fengtian,Wu Ling
The process of hydrogen bond donor accelerating the cycloaddition of epoxides with CO2 is green access to high economic value cyclocarbonate derivatives. However, hydrogen bond donor still has certain limitations such as poor biocompatibility and narrow substrate
scope. Our group found that folic acid could promote the coupling reaction of epoxides and CO2 through hydrogen-bonding. The reaction was used to synthesize various cyclocarbonate derivatives in good to high yields with the aid of folic acid and TBAB. In addition, benzoic
acids and 2,4-quinazoline dione were synthesized in the presence of CuCl2/folic acid and PdCl2/folic acid, respectively. The reaction mechanism was proposed based on previous reports and control experiments.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2017
·Vol. 28
·期 24
·18735-18744
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IF 2.019
Zhang Wei,Wu Weihong,Qu Hongqiang,Xu Jianzhong,Ye Leilei,Li Baoming
In this paper, a facile method was introduced to prepare the hierarchical composite that the aligned Co 2+ doped PANI nanowires and twining Co 2+ doped PANI nanofibers were delicately synthesized on the graphite fiber (Co 2+ doped PANI/gf). The structure of Co 2+ doped PANI was confirmed by Fourier transform infrared spectroscopy and X-ray photoelectron survey. The scanning electron microscopy showed that the surface morphology of Co 2+ doped PANI/gf could be controlled by adjusting the molar ratio of An/Co 2+ and the aniline concentration. The Co 2+ doped PANI/gf hierarchical composite exhibited a high specific capacitance of 562 F/g at 0.2 A/g and presented excellent cycling durability that it retained 92.9% of the initial specific capacitance after 1000 cycles at a scan rate of 100 mV/s. The improved electrochemical performance suggested a promising application of the Co 2+ doped PANI/gf hierarchical composite in high performance supercapacitor.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2025
·
IF 2.2
Jing Xia,Zhigao Sun
Hydrate inhibitors can effectively prevent hydrate blockage in pipelines. Thermodynamic inhibitors suppress hydrate formation by altering hydrate phase equilibrium conditions. This paper primarily investigates the influence of 1,2,4-Triazole aqueous solutions at different concentrations on carbon dioxide hydrate dissociation conditions by the graphical method. 1,2,4-triazole can enhance hydrate formation pressure. With higher concentrations of 1,2,4-triazole, it has a stronger inhibitory influence on carbon dioxide hydrates. Compared to methanol and ethylene glycol, 1,2,4-triazole exhibits lower toxicity and better biodegradability, making it an environmentally friendly hydrate thermodynamic inhibitor. The nitrogen atoms in the molecular structure of 1,2,4-triazole possess polarity, enabling them to form strong hydrogen bond. This enhances competition for water molecules, decreasing the water for hydrate formation and consequently inhibiting hydrate nucleation.
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Nature Communications
·
2025
·Vol. 16
·期 1
·10727
·
IF 15.7
Wang Sifan,Fang Zhecheng,Yu Can,Li Bolong,Wang Jianghao,Zhang Jiaji,Zhang Zihao,Zhou Wenhua,Yao Siyu,Song Weiyu,Liu Zhao-Qing,Cheng Dangguo,Fu Jie
Electrocatalytic reduction of CO 2 to ethylene utilizing Cu-based catalysts in acidic media demonstrates considerable potential for addressing energy and environmental challenges. However, cationic Cu δ+ is apt to be reduced to Cu 0 under the harsh acidic CO 2 reduction conditions. Here we show that the interface of yttrium-doped ZrO 2 and CuO (YSZ/CuO) can stabilize cationic Cu δ+ , preventing its over-reduction even at high applied potentials. The YSZ/CuO catalyst achieves a faradaic efficiency of 68.7% and a partial current density of 545.0 mA·cm –2 for ethylene formation in acidic media (pH = 2). In-situ characterization and theoretical calculations indicate that the abundant oxygen vacancies in YSZ promote the initial formation of interfacial oxygen from CuO rather than the support . The interfacial oxygen derived from CuO offers a high charge density of Cu, facilitated by electron transfer from Zr/Y to Cu, leading to a shortened Cu-O bond and enhances stabilization against reduction. This interface engineering strategy not only protects cationic metals under reducing and acidic conditions but also provides valuable insights applicable across heterogeneous catalysis.
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