INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2013
·Vol. 38
·期 13
·5251-5258
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IF 3.548
Qiang Zhao,Zhuobin Yu,Wen Yuan,Jinping Li
Under mild conditions (near-neutral aqueous solutions, room temperature , and atmospheric pressure), an attractive electrolyte was expanded for splitting water and three novel oxygen-evolution catalysts (Co-C i , Ni-C i , Ag-C i ) were generated. The Co-C i catalyst showed a high oxygen-evolution rate (24.42 μmol h −1 ), a low oxygen-evolution overpotential (395 mV) and excellent stability. In addition, the non-amorphous Ag-C i catalyst, different from reported catalyst, was generated. The catalyst has been further characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive spectrometry (EDS), and X-ray photoelectron spectroscopy (XPS).
研究领域:
材料化学
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电化学
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催化化学
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能源科学
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纳米材料
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Di Li,Jing Yang,Hao Chen,Hongxin Guan,Sheng Chen,Qiang Li,Jingjing Duan
Matched, oriented and fast local proton and electron supply are vital for industrial-level eCO 2 RR. • Modifying Cu catalysts using conductive functionalized polymers, could finely modulate proton and electron transport. • Methyl groups repel water and confine CO 2 , *CO intermediates nearby Cu, suppress HER and augment carbon-carbon coupling. A b s t r a c t Electrocatalytic CO 2 reduction reaction (eCO 2 RR) is an effective solution for environmental and energy crises caused by excessive CO 2 emission, consisting of multiple proton-coupled electron transfer (PCET) steps. Especially, to achieve industrial-level current densities, oriented and fast proton and electron supply is critical while challenging due to hydrogen evolution by-reaction (by-HER). In this work, functionalized conductive polymers are utilized to modify the traditional Cu-based gas diffusion electrode (GDE) regulating both local electron and proton transport for eCO 2 RR. Among which, pyrrole-3-methyl (PPy-3-CH 3 ) modified Cu-GDE has achieved an excellent Faradaic efficiency for double-carbon (C 2 ) products above 80.0% in a wide working range of 300–600 mA cm −2 , due to its moderate activation energy barrier for electron and proton conduction. Specifically, the electron and proton transport via the facile Grotthuss mechanism, whose energy barriers are lower than the Vehicle mechanism. Furthermore, -CH 3 groups could repel water, confine CO 2 reactants and *CO intermediates nearby Cu catalytic sites, suppressing by-HER and augmenting carbon-carbon coupling. However, -COOH groups also act as proton hopping sites except -NH groups, increasing local protons and thus severe by-HER. This work underscores importance of matched local electron-proton supply for electrocatalysts during PCET mediated electrocatalytic reaction, facilitating their industrial success. Download: Download high-res image (247KB) Download: Download full-size image Fast, oriented and matched proton and electron supply is developed by modifying the cupper based electrocatalyst using conductive polymers with different functional groups at various positions, therefore, achieving an industrial-level process of electrochemical CO 2 reduction to multi-carbon products.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Xuebi Du,Huan Zeng,Qi Gao,Chen Li,Yin Quan,Lihua Chen,Shichao Feng,Yinhua Wan
In this study, the morphology of ZnO was altered from nanofibers to hollow nanotubes by Ce doping, mainly owing to the Kirkendall effect originating from different diffusion rates of constituent elements. A novel one-dimensional core-shell nanotube (ZnO-CeO 2 @ZIF-8) was successfully fabricated, characterized by a distinctive structure comprising a ZIF-8 shell and a ZnO-CeO 2 nanotube core. The as-prepared ZnO-CeO 2 @ZIF-8 exhibited a large specific surface area, substantial pore volume, and strong affinity towards CO 2 . These ZnO-CeO 2 @ZIF-8 were integrated into Pebax-1657 to construct MMMs for high-efficiency CO 2 transport and separation. Furthermore, the unique 1D hollow structure of the filler effectively reduced the resistance to mass transfer and enhanced gas permeability, while the ZIF-8 shell and Ce-induced oxygen vacancies synergistically enhanced the CO 2 adsorption and selectivity. The Pebax/ZnO-CeO 2 @ZIF-8 MMMs containing 3 wt% loading demonstrate superior performance, characterized by a CO 2 permeability of 94.0 Barrer and CO 2 /N 2 selectivity of 64.8 respectively. Compared to the unmodified Pebax, these values exhibit enhancements of 73.4% and 36.7%, suggesting that ZnO-CeO 2 @ZIF-8 holds considerable promise in the realm of MMMs for adsorption and separation of CO 2 .
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
·Vol. 30
·期 18
·51876-51886
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IF 5.8
Yu Weiting,Zhu Jieyun,Chen Sizhuo,Tang Juntao,Ye Jiexu,Song Shuang
The electrocatalytic reduction of CO 2 towards CO is one of the most desirable routines to reduce atmospheric CO 2 concentration and maintain a global carbon balance. In this work, a novel porous NiCu-embedded ZIF-derived N-doped carbon nanoparticle (NiCu@NCNPs) catalyst has been identified as an active, highly selective, stable, and cost-effective catalyst in CO 2 reduction. A CO selectivity as high as 100% has been achieved on NiCu@NCNPs which is the highest reported to date. The particle current density of CO on NiCu@NCNPs is around 15 mA cm –2 under the optimized potential at −0.9 V vs. RHE. The NiCu@NCNPs electrode also exhibits excellent stability during the five sequential CO 2 electroreduction experiments. The superior catalytic performance of NiCu@NCNPs in CO 2 RR can be related to its microstructure with high electrochemical surface area and low electron transfer resistance. Furthermore, a kinetic analysis has shown the formation of intermediate *COOH is the rate-determining step in CO 2 RR towards CO. According to the results of density functional theory (DFT) calculations, a low Gibbs-free energy change (∆ G ) for the rate-determining step leads to the enhanced catalytic performance of CO 2 RR on NiCu@NCNPs.
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ENERGY
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2023
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IF 9
Yunzhao Guo,Huiping Zhang,Kaiyun Fu,Xianfu Chen,Minghui Qiu,Yiqun Fan
Amine-based absorption has matured into an established technology for CO 2 capture from fossil fuel power plants. However, high energy consumption for CO 2 desorption remains a challenge. Herein, we report a promising integration of a solid acid catalyst (i.e., HZSM-5) filled into a vapor permeable-liquid impermeable tubular α-Al 2 O 3 ceramic membrane for boosting CO 2 desorption from aqueous monoethanolamine (MEA) solution. Experiments were conducted to investigate the effects of catalyst weight, temperature, pressure, liquid flow rate and CO 2 loading on CO 2 desorption rate and energy consumption. Furthermore, 60 runs of cyclic tests were carried out to assess the stable CO 2 desorption rate and the thermal and chemical stability of both the HZSM-5 catalyst and the α-Al 2 O 3 membrane. The experiment results demonstrated that the HZSM-5 filled α-Al 2 O 3 ceramic membrane contactor exhibited high CO 2 desorption performance and long-term stability. It is anticipated that integration of solid acid catalyst with porous ceramic membrane holds great promise in practical application to boost the CO 2 desorption rate and reduce the energy requirement.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2023
·Vol. 27
·期 5
·1261-1268
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IF 2.5
Deng Hao-chen (Preston),Hao Qingzhu,Wang Yuhang
The COVID-19 pandemic that is still prevalent around the globe each day consumes massive disposable face masks and consequently lays a heavy burden on waste management. Meanwhile, the incineration of these medical wastes further escalates the already overwhelming carbon emission that leads to global warming and climate change. To offer a potential solution addressing medical waste and CO 2 emission challenges, we herein develop a synthetic protocol to upgrade face masks into Ni, N-doped graphene (Ni–N-C) sheet catalysts for selectively reducing CO 2 into CO electrochemically. The high specific surface area and the uniform dispersion of Ni active sites of the catalyst derived from a regular disposable face mask enable a near-unity CO Faradaic efficiency (FE) at the current density of 200 mA cm −2 . This study offers outside-of-the-box thinking to address environmental issues by turning medical wastes into CO 2 reduction catalysts.
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INORGANIC CHEMISTRY
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2023
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IF 4.6
Shanshan Wu,Meng Tian,Yang Hu,Nan Zhang,Wei Shen,Jianyi Li,Linchuan Guo,Pengfei Da,Pinxian Xi,Chun-Hua Yan
Formate is identified as economically viable chemical fuel from electrochemical carbon dioxide reduction. However, the selectivity of current catalysts toward formate is limited by the competitive reaction such as HER. Herein, we propose a CeO2 modification strategy to improve the selectivity of catalysts for formate through tuning of the *OCHO intermediate, which is important for formate production.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Wenjian Yue,Xiaojiang Li,Junhao Jing,Jie Qi,Shanshan Dai,Hongsheng Lu,Zhiyu Huang
Hydrocarbon pollutants are not only serious environmental hazards in the exploitation of petroleum resources, but also lead to incomplete utilization of resources. At present, a green solvent called deep eutectic solvents (DES) gradually replaces traditional organic solvents to recover petroleum hydrocarbons, but its recovery still needs to be optimized. For this reason, hydrophobic DES with hydrophilic and hydrophobic properties that can be controlled by CO 2 was developed using fatty acid (FA) as raw material. In the process of using liquid FA to drop into solid FA to prepare DES with an adjustable melting point, DCS technology was used to accurately obtain the melting point and latent heat of the experimental reagent FAs, and the solid − liquid diagram of DES was predicted. Interestingly, the DES prepared by the addition of solid FA and liquid FA retains its strong hydrophobic properties, while the viscosity and melting point can be significantly reduced. FA can transform from oil-soluble physical property to water-soluble physical property by electrostatic binding to polyether amine (D230). This weak non-covalent bond force can be dissociated by CO 2 stimulation, FA can be restored to oil-soluble state, and D230 in aqueous phase can be reduced by removing CO 2 by heating or bubbling N 2 . The reversible pH transformation of the system and 1 H NMR confirm this CO 2 -switchable behavior. In addition, sustainable oil separation (kerosene) was successfully achieved with a maximum oil recovery of 94.6%. Therefore, the novel FA-based DES is expected to be used as an effective extractant for the sustainable clean recovery of hydrocarbons from petroleum resources.
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MOLECULES
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2023
·Vol. 28
·期 5
·2272
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IF 4.6
Zhangxi Gao,Mei Xiang,Mingyang He,Weiyou Zhou,Jiayao Chen,Jiamin Lu,Zeying Wu,Yaqiong Su
Catalytic conversion of CO2with the surplus glycerol (GL) produced from biodiesel manufacturing has attracted much academic and industrial attention, which proves the urgent requirement for developing high-performance catalysts to afford significant environmental benefits. Herein, titanosilicate ETS-10 zeolite-based catalysts with active metal species introduced by impregnation were employed for coupling CO2with GL to efficiently synthesize glycerol carbonate (GC). The catalytic GL conversion at 170 °C miraculously reached 35.0% and a 12.7% yield of GC was obtained on Co/ETS-10 with CH3CN as a dehydrating agent. For comparison, Zn/ETS- Cu/ETS-10, Ni/ETS-10, Zr/ETS-10, Ce/ETS-10, and Fe/ETS-10 were also prepared, which showed inferior coordination between GL conversion and GC selectivity. Comprehensive analysis revealed that the presence of moderate basic sites for CO2adsorption-activation played a crucial role in regulating catalytic activity. Moreover, the appropriate interaction between cobalt species and ETS-10 zeolite was also of great significance for improving the glycerol activation capacity. A plausible mechanism was proposed for the synthesis of GC from GL and CO2in the presence of CH3CN solvent over Co/ETS-10 catalyst. Moreover, the recyclability of Co/ETS-10 was also measured and it proved to be recycled at least eight times with less than 3% decline in GL conversion and GC yield after a simple regeneration process through calcination at 450 °C for 5 h in air.Keywords:CO2;glycerol;glycerol carbonate;ETS-10 zeolite;cobalt-based catalyst
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Sihui Li,Keming Zhang,Chenlu Liu,Xiaoting Feng,Peijin Wang,Shaofei Wang
Polymeric membranes containing polyethylene oxide (PEO) groups are promising CO 2 separation materials, but suffer from the trade-off between separation performance and mechanical strength . To overcome this challenge, we combine the merits of semi-interpenetrating polymer network and nanohybrid to maintain a high PEO loading and robust membrane structure. The membranes were prepared by introducing in-situ formed PEO networks with silica nodes into Pebax1657 to produce a semi-interpenetrating network structure. The introduced network and in situ formed silica nanoparticles reduce the chain packing efficiency of Pebax matrix to enhance the CO 2 diffusivity , while the increased PEO content enhances CO 2 solubility. Under feed gas pressure of 25 bar, nanohybrid membranes containing 40 wt% polymer network display excellent gas separation performance with CO 2 permeability of 272.8 Barrer and CO 2 /N 2 selectivity of 79.6 under mixed gas separation tests, surpassing 2008 Robeson upper bound. Moreover, the hybrid membranes showed high mechanical strength, the Young's modulus increases by 1.95 times. This strategy provides a simple route for the design of nanohybrid membranes with high separation performance as well as excellent durability.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Ruolin Cheng,Anhu Wang,Shuxun Sang,Huagen Liang,Shiqi Liu,Panagiotis Tsiakaras
The CO 2 cycloaddition of epoxides is a highly attractive long-term carbon fixation strategy, but harsh reaction conditions and expensive catalytic materials limit its industrial application. Herein, low-cost and highly efficient W 18 O 49 -based composites were constructed by in-situ solvothermal synthesis. It is found that W 18 O 49 /g-C 3 N 4 composites exhibit the highest yield of 74% (271 mmol g −1 h −1 ) in the probing reaction of styrene carbonate production. The physicochemical characterizations indicate that the photocatalysis plays a fundamental role in this reaction by promoting the activation of CO 2 and styrene oxide. The crucial role of photogenerated electrons and Lewis acid-base sites is confirmed. In this work, a novel catalyst selection to produce cyclic carbonate under ambient conditions is presented.
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Journal of Physical Chemistry C
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2023
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IF 3.7
Yuchen Zhou,Yu Wang,Zezhi Chen,Huijuan Gong,Lu Chen,Huiqiang Yu
Carbonic anhydrase (CA) is an enzyme with unparallele d catalytic activity in CO2 hydration. However, its high cost and low stability seriously restrict its industrial application in CO2 absorption. Constructing CA mimics is a promising strategy to overcome the above limitations. However, to date, a majority of mimics reported are suffering from laborious synthetic processes, harsh synthetic conditions, and costly ligand materials. Therefore, developing novel CA mimics with higher applicability remains a high priority. Due to the structural similarity between zeolite imidazolate framework (ZIF)-8 and natural carbonic anhydrase (CA), ZIF-8 may be considered as a potential CA-mimetic catalyst for CO2 absorption. To validate this assumption, ZIF-8 and hydrophilic ZIF-8-TA were synthesized and the results from subsequent CO2 absorption experiments indicated that the synthesized catalysts could significantly enhance CO2 absorption in water and common alkaline solutions. The addition of 1.0 wt % ZIF-8 in water and different alkaline solutions respectively increased the average CO2 absorption rate by 42.35 and 6.78–24.51%, while the addition of 1.0 wt % of ZIF-8-TA increased the CO2 absorption rate by 81.80 and 18.16–34.39%, respectively. Besides, both catalysts possessed excellent reusability that they retained high performance even after five cycles of absorption and regeneration. Through esterase experiments, it was confirmed that ZIF-8 and ZIF-8-TA exhibited higher CA-mimetic activity than many reported CA mimics. Through density functional theory (DFT) calculations, it was indicated that the catalytic CO2 hydration pathway of ZIF-8 primarily involves four steps, including nucleophilic attack, rearrangement, replacement, and deprotonation, which is similar to that of natural CA, while ZIF-8-TA does not undergo the rearrangement step. Moreover, the electron-donation effect and van der Waals interaction of tannic acid endow ZIF-8-TA with higher catalytic activity.
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