MATERIALS RESEARCH BULLETIN
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2019
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IF 3.355
Xiya Wang,Zhaoguo Zhang,Zhengfeng Huang,Peimei Dong,Xiaoxiao Nie,Zhi Jin,Xiwen Zhang
The photoreduction of CO 2 by using Ho and N co-doped TiO 2 was explored. The doping elements can further improve the separation efficiency of photogenerated electron-hole pairs via refining grains, causing lattice distortion and adsorbing more hydroxyl radicals(·OH). We found that there exists product selectivity such that the photoreduction products of Ho/N-TiO 2 mainly consist of CO and methanol, while the counterparts of pristine TiO 2 are CO and methane. The possible mechanism of CO 2 reduction is depicted involving the generation and combination of specific radicals. Thus, the amount of ·OH adsorbed on the surface of the catalyst makes a significant difference in the selectivity in the reduction products. Ho/N-TiO 2 catalyst with the synergic effect of Ho and N showed the best photoreductive performance for CO 2 with H 2 O to CO and CH 4 , and its formation rate of CH 4 was 29 μmol/gcatal./hour.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
·
IF 3.375
Qingqing Li,Yanxing Zhang,Xurui Zhang,Hongqiang Wang,Qingyu Li,Jiawei Sheng,Jin Yi,Yuyu Liu,Jiujun Zhang
Electrochemical reduction of CO2 to useful low-carbon fuels can not only mitigate global warming problems but also be used for energy storage. For efficient CO2 electrochemical reduction in mild conditions, high-performance catalysts are required. In this work, the electrodeposition of bismuth, tin, or both on copper sheets to fabricate Sn/Cu, BiSn/Cu, Bi2Sn/Cu, Bi3Sn/Cu, Bi4Sn/Cu, and Bi/Cu electrodes was conducted, and the electrodes were used as catalysts in CO2 reduction. Experimental results show these electrodes have high activity, stability and selectivity toward CO2 reduction to formic acid. A maximum Faraday efficiency of 90.4% for formic acid production can be achieved when using a Bi/Cu electrode. The mechanism catalyzed by such electrodes is also proposed for fundamental understanding and is clearly explained on the basis of DFT calculations. The results in this paper demonstrate that electrodeposition can be a faster and easier to operate industrial technology for the fabrication of catalyst electrodes, compared with other technologies.
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ELECTROCHIMICA ACTA
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2019
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IF 5.383
Jianzhi Huang,Lishi Wang
In this work, we first discover the new bifunctional abilities of wood for highly selective electrocatalytic CO 2 reduction to formate and highly sensitive electroanalytical detection of myricetin and cadmium (II). The highly developed microchannels in wood ensure most effective reactant and electrolyte transport, great facilitating the electrode reaction . The activated wood electrode displays excellent electrocatalytic CO 2 reduction activity, attained the highest formate Faradaic Efficiency (FE) of 70.8% at −1.8 V with high current density of 53.8 mA cm −2 in aqueous solution, and displayed at least 24 h CO 2 electrolysis durability. Furthermore, the wood is also first utilized as new electrode matrix for electroanalytical detection of drug (myricetin is as an example) and heavy metal ion (cadmium (II) is as an example). Compared with traditional glassy carbon electrode (GCE) and its derived modified electrodes , the wood electrode exhibits a wide linear detection range (0.01–50 μmol dm −3 ) and a low detection limit (0.002 μmol dm −3 , S/N = 3) for myricetin , and displays a wide linear detection range (0.1–20 μg l −1 ) and a low detection limit (0.05 μg L −1 , S/N = 3) for cadmium (II). These remarkable bifunctional performances of low cost wood electrode show great potential for large-scale using in CO 2 electroreduction and electroanalytical detection.
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ACS Catalysis
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2019
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IF 12.221
Chao Hu,Silin Bai,Lijun Gao,Sucen Liang,Juan Yang,Shao-Dong Cheng,Shao-Bo Mi,Jieshan Qiu
Metal-doped zeolitic imidazolate framework-8 (ZIF-8)-derived carbon materials are attractive for the electrocatalytic reduction of CO2 into CO. In such carbon materials, due to the fusion and aggregation of ZIF-8 precursors during the high-temperature pyrolysis process, it is desirable yet still challenging to create a high specific surface area with more active sites available for reacting with reactants. Using SiO2 as a protective coating on the ZIF-8 surface, we synthesize Fe, N-co-doped porous carbon nanoparticles (Fe-CNPs) which possess a hierarchical pore structure with a specific surface area as high as 1156.6 m2 g–1, much higher than the counterparts without a SiO2 coating (360.1 m2 g–1). Over these highly porous Fe-CNPs, the total current densities are more than 3 times higher than those of the lowly porous ones for the electrochemical CO2 reduction. More importantly, the maximum CO Faradaic efficiency for Fe-CNPs increases from ca. 75.0 to 98.8% in a concentrated KHCO3 solution (1 mol L–1). The porosity-induced high selectivity for CO production is also revealed on Ni-doped and Co-doped ZIF-derived CNPs, suggesting a new pathway for designing high-performance carbon catalysts through engineering the porosity for the electrochemical CO2 reduction.
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ENVIRONMENTAL POLLUTION
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2019
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IF 5.714
Fang Dong,Pu Wang,Wei Qian,Xing Tang,Xiaoshan Zhu,Zhenyu Wang,Zhonghua Cai,Jiangxin Wang
Ocean acidification (OA) is a global problem to marine ecosystems . Cadmium (Cd) is a typical metal pollutant, which is non-essential but extremely toxic to marine organisms. The combined effects of marine pollution and climate-driven ocean changes should be considered for the effective marine ecosystem management of coastal areas. Previous reports have separately investigated the influences of OA and Cd pollution on marine organisms. However, little is known of the potential combined effects of OA and Cd pollution on marine diatoms. We investigated the sole and combined influences of OA (1500 ppm CO 2 ) and Cd exposure (0.4 and 1.2 mg/L) on the coastal diatom Skeletonema costatum . Our results clearly showed that OA significantly alleviated the toxicity of Cd to S. costatum growth and mitigated the oxidant stress, although the intercellular Cd accumulation still increased. OA partially rescued S. costatum from the inhibition of photosynthesis and pyruvate metabolism caused by Cd exposure. It also upregulated genes involved in gluconeogenesis, glycolysis, the citrate cycle (TCA), Ribonucleic acid (RNA) metabolism, and especially the biosynthesis of non-protein thiol compounds. These changes might contribute to algal growth and Cd resistance. Overall, this study demonstrates that OA can alleviate Cd toxicity to S. costatum and explores the potential underlying mechanisms at both the cellular and molecular levels. These results will ultimately help us understand the impacts of combined stresses of climate change and metal pollution on marine organisms and expand the knowledge of the ecological risks of OA.
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JOURNAL OF MEMBRANE SCIENCE
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2019
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IF 7.015
Chenhui Wang,Fangyuan Guo,He Li,Jian Xu,Jun Hu,Honglai Liu,Meihong Wang
Inspired by the most efficient CO 2 transport across natural biological membranes , a novel bionic channel facilitating CO 2 permeation was realized via adding a filtering porous ionic polymer (PIP) in a mixed matrix membrane (MMM). A series of polymer of intrinsic microporosity (PIM-1) based MMMs were fabricated by three pyridine-based PIPs (PIP-Py-X) with different Cl − , Ac − , and BF 4 − anions as fillers. PIP-Py-X PIPs show highly selective CO 2 adsorption capacity and perfect interfacial compatibility with the PIM-1 matrix. More significantly, acting as carriers, the movable anions in the MMMs efficiently facilitated the transport of adsorbed CO 2 across the membranes. As a result, the obtained PIM-Py-Ac-15 MMM exhibited an excellent permeability for CO 2 of 6205 barrer and a CO 2 /N 2 and CO 2 /CH 4 selectivity of 62.5 and 56.1, respectively, far surpassing the 2008 Robeson upper bound and exceeding most of the reported advanced membranes. As a divertive of PIPs, this work opens a window for designing and fabricating promising MMMs for task-specific membrane separations .
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JOURNAL OF MEMBRANE SCIENCE
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2019
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IF 7.015
Mingmin Jia,Xiong-Fei Zhang,Yi Feng,Yichen Zhou,Jianfeng Yao
ZIF-8@cellulose nanofiber (ZIF-8@CNF) composite membranes were prepared via in-situ growing ZIF-8 crystals on cellulose nanofibers (CNFs) and vacuum filtration. Owning to the electrostatic forces between –COO - of CNFs and Zn 2+ of ZIF-8, ZIF-8 crystals were anchored homogenously on CNFs. With ZIF-8 loading increased to sufficiently high, the intrinsic selectivity of ZIF-8 played an important role for gas separation. As a result, the optimum separation performance is achieved over ZIF-8@CNF-70 composite membrane with CO 2 permeability of 550 Barrer and CO 2 /N 2 and CO 2 /CH 4 ideal selectivity of 45.5 and 36.2, respectively.
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FUEL
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2018
·
IF 4.908
Haiyang Tian,Hongping Quan,Zhiyu Huang,Silong Jiang
The non-hydrophobically associating water-soluble polymer (DPAM) of acrylamide (AM) and dimethylamino propyl methacrylamide (DMAPMA) was synthesized. Then pH-switchable and CO 2 ‑switchable viscoelastic liquids based on DPAM and anionic surfactant sodium dodecyl sulfate (SDS)(referred to as DPAM-SDS) were developed. When minor HCl aqueous solution was added into the DPAM and SDS aqueous mixture or CO 2 was bubbled into it, the tertiary amine groups of DPAM were protonated to form quaternary ammonium groups, some of which in the same quaternary ammonium groups of DPAM “bridged” some SDS through noncovalent electrostatic attraction, behaving like a pseudo-hydrophobically associating water-soluble polymer and forming viscoelastic fluids as checked through environmental scanning electron microscope(ESEM) and rheology. Upon removing of CO 2 or back of pH by minor NaOH aqueous solution, the quaternary ammonium species of DPAM were deprotonated back to tertiary amine groups, separating the pseudo-hydrophobically associating water-soluble polymer back to DPAM and SDS molecules, which resulted in forming low-viscosity water solution. The switchable viscoelastic conversion can be repeated.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Yazhi Yin,Bing Hu,Xinliang Li,Xiaohai Zhou,Xinlin Hong,Guoliang Liu
Direct CO 2 hydrogenation to methanol provides a means of CO 2 fixation and a way of hydrogen storage in a more energy-dense and transportable form. Pd-ZnO catalysts can be active for this reaction, but their activities are strongly associated with the preparation methods which influence the dispersion and stability of Pd nanoparticle. Here we report a novel fabrication of highly effective PdZn alloy catalysts derived from Pd@zeolitic imidazolate framework (ZIF-8) for the hydrogenation of CO 2 . The confinement of subnanometric Pd particles in the pore framework of ZIF-8 facilitates the formation of Pd-ZnO interfaces with strong-metal-support-interaction (SMSI) after a simple pyrolysis under air condition. The porous texture and high surface area of ZnO ensures a high dispersion of Pd nanoparticles. Different pyrolysis temperatures were studied in catalysis and the highest methanol yield reached 0.65 g g cat −1 h −1 at 270 °C, 4.5 MPa, with a TOF of 972 h −1 , over a PdZn catalyst prepared at 400 °C. Such excellent activity has ranked the top reported values over advanced Pd-based catalysts under comparable conditions. The crucial factors for such high methanol yield are the formation of small-sized PdZn alloy particles after H 2 reduction and abundant surface oxygen defects on ZnO. The SMSI between PdZn and ZnO also ensures a long term stability of our PdZn catalysts. At last, we propose the active site that was strongly associated with methanol formation is a PdZn alloy rather than metallic Pd.
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Catalysts
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2018
·Vol. 9
·期 1
·16
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IF 3.465
Yuehong Yu,Jiaxiang Qin,Min Xiao,Shuanjin Wang,Dongmei Han,Yuezhong Meng
Introducing mesopores into the channels and cages of conventional micropores CHA (Chabazite) topological structure SAPO-34 molecular sieves can effectively improve mass transport, retard coke deposition rate and enhance the catalytic performance for methanol to olefins (MTO) reaction, especially lifetime and olefins selectivity. In order to overcome the intrinsic diffusion limitation, a novel CO2-based polyurea copolymer with affluent amine group, ether segment and carbonyl group has been firstly applied to the synthesis of SAPO-34 zeolite under hydrothermal conditions. The as-synthesized micro-mesoporosity SAPO-34 molecular sieve catalysts show heterogeneous size distribution mesopores and exhibit slightly decrease of BET surface area due to the formation of defects and voids. Meanwhile, the catalysts exhibit superior catalytic performance in the MTO reaction with more than twice prolonged catalytic lifespan and improvement of selectivity for light olefins compared with conventional microporous SAPO-34. The methodology provides a new way to synthesize and control the structure of SAPO-34 catalysts.Keywords:molecular sieves;SAPO-34;MTO;CO2-based polyuria;mesoporogen
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ACS Applied Materials & Interfaces
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2018
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IF 8.097
Fangfang Yang,Mian Wu,Yuchao Wang,Saeed Ashtiani,Heqing Jiang
Metal–organic framework (MOF) nanosheets have emerged as promising materials for the construction of molecular sieve membranes due to their nanoscale thickness and highly oriented pore arrays. However, the development of defect-free MOF nanosheet membranes from rigid MOF nanosheets with efficient permselectivity and robust mechanical strength still remains a big challenge. Herein, we develop a facile GO-induced assembly strategy to design continuous and uniform two-dimensional MOF composite membranes, in which the copper 1,4-benzene dicarboxylate (CuBDC) nanosheets present a layer-stacking arrangement. With the assistance of flexible GO, the voids between the junctions of rigid MOF nanosheets are well-repaired, and the interlayer bonding interactions are strengthened, resulting in the fabrication of a continuous nanosheet membrane with robust mechanical strength. The obtained MOF nanosheet-based membranes display remarkable H2/CO2 separation performance with a superior H2 permeance of 9.6 × 10–7 mol m–2 s–1 Pa–1 and an ideal separation selectivity of 95.1 due to the well-defined size exclusion effect, showing great promise for H2 separation and purification. The repair strategy described here could also provide the blueprint for the development of other nanosheet-based membranes.
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CATALYSIS LETTERS
·
2018
·Vol. 148
·期 7
·1827-1833
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IF 2.911
Xu Weina,Wang Zheyu,Chen Gong,Fu Zhongwang,Jiang Guoqiang,Chen Jian,Wu Jianzhong,Liu Zheng
Abstract We report a facile method for encapsulation of carbonic anhydrase (CA) with magnetic nanogel (MNP-CA nanogel), in which amino and vinyl groups are first grafted onto the surface of magnetic Fe 3 O 4 nanoparticles (MNP) using 3-aminopropyltriethoxysilane (APTES) and N -acryloylsuccinimide (NAS), followed by CA attachment with glutaraldehyde and in situ polymerization with acrylamide. The MNP-CA nanogel shows much improved thermostability at elevated temperatures, e.g. staying unchanged at 60 °C for 80 min, owing to multiple linkage with the hydrophilic polymer network coated at the MNP surface. Addition of the MNP-CA nanogel into a methyldiethanolamine (MDEA) solution at an ultralow mass ratio (1:10 4 ) is able to enhance the CO 2 absorption rate at 60 °C by 1.45 fold. The CA-enhanced mass transport of the absorbate has been demonstrated in a wetted-wall column, in which the MNP-CA nanogel increases the total mass transfer coefficient in the gas phase (K G ) by 4.61 fold compared with that determined in the MDEA solution. The greatly increased absorption performance and much enhanced stability make MNP-CA nanogel appealing for industrial applications. Graphical Abstract
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