ChemCatChem
·
2023
·Vol. 15
·期 4
·e202201413
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IF 4.5
Dandan Zhao,Shaoyang Zhang,Tianyu Guo,Qiang Zhao,Jianping Du,Jinping Li
Graphical Carbon dioxide reduction : The rectangular nanoflakes with crystalline/amorphous phase structures that the square nanoblocks are confined in amorphous nanoflakes efficiently enhance the electrocatalytic conversion of CO 2 to ethylene. The electrocatalytic reduction of CO 2 to high value-added chemicals is one of the effective technologies to achieve the goal of carbon neutralization. However, highly selective production of hydrocarbon via electrochemical conversion of CO 2 still has great challenges. Herein, a unique CuO phase composition is constructed that consists of rectangular nanoflakes possessing crystalline/amorphous structures by the facile strategy. Crystalline CuO square nanoblocks are confined in amorphous nanoflakes and form crystalline/amorphous hybrid phase. The results of electrocatalytic CO 2 reduction demonstrate that this crystalline/amorphous CuO material exhibits superior CO 2 conversion ability with ethylene Faradaic efficiency of 58.3 % at −1.08 V vs. RHE, which is ascribed to nanoflake structures and fast electron transfer on the crystalline/amorphous interfaces because of superior conductivity of amorphous CuO. The present research provides an effective route to reconstruct novel crystalline/amorphous interfaces of CuO for catalysis applications.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Yanzheng Ji,Xingyu Liu,Haochen Li,Xuan Jiao,Xinquan Yu,Youfa Zhang
The performance of activated carbon (AC) will be severely affected for carbon dioxide (CO 2 ) capture in flue gas, as they usually suffer from competitive adsorption of water vapor. Establishment of a barrier against moisture on the surface of porous adsorbent material could potentially address this issue. Zeolite-like metal–organic frameworks (ZIF-8) as a promising adsorbent material demonstrates hydrophobic properties, large specific surface area, and highly porous structure. Here, by further growth of ZIF-8 on polydopamine (PDA)-coated bio-based carbon (AC@PDA), we fabricate hydrophobic final product (AC@ZIF-8). The CO 2 capture capacities of AC@ZIF-8 was 41.69 cm 3 /g, which is only 13.61% lower than that of the initial AC under dry conditions. The hydrophobic ZIF-8 layer can effectively prevent water molecules from reaching the interior AC. Therefore, the adsorption of CO 2 for AC@ZIF-8 decreased by only 16.74% under high relative humidity, while it decreased by 61.27% for bare AC. This strategy will broaden the applications of carbon-based adsorbents for CO 2 capture under severely humid conditions. We believe that this approach is also applicable for an extensive set of CO 2 capture materials that suffer from water instability.
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TOPICS IN CATALYSIS
·
2023
·Vol. 66
·期 19
·1527-1538
·
IF 3.6
Zhang Li,Men Yong,Wu Bin,Feng Yuanfen,Song Chao,Liu Shuang,Wang Jinguo,An Wei,Magkoev Tamerlan T.
Highly selective production of valuable ethylene from electrocatalytic CO 2 reduction reaction (ECO 2 RR) is particularly desirable yet challenging. Morphology engineering is an effective strategy for catalyst design, which can adjust the electronic structure of catalyst surface, change the adsorption behavior of critical reaction intermediates over catalyst surface, and thus regulate the activity of electrocatalytic CO 2 reduction reaction. In this work, we prepared copper phosphate catalysts with different morphologies and tested their catalytic activity for the ECO 2 RR in the flow cell. Compared with irregular flocculent aggregates, copper phosphate nanospheres exhibit a high and stable ethylene Faradaic efficiency of 47% with high current density of 350 mA·cm − 2 , which is higher than the 200 mA·cm − 2 required for industrial applications. The catalysts were extensively characterized by SEM, EDS, XRD, ICP-OES, XPS, BET and CO-TPD. Combining the characterization results and activity data, we found that the superior spherical morphology of copper phosphate can increase the electron density around Cu, stabilize the Cu + species on the surface through the electron transfer between P and Cu, and adjust the adsorption strength of CO intermediates (*CO) to enhance the productivity of C 2+ products. This work provides new insights into catalyst design for highly efficient C 2 H 4 production from the electrocatalytic CO 2 reduction reaction by tuning morphologies of Cu-based catalysts.
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Yuehui Li,Duanhui Si,Wangyin Wang,Song Xue,Wenzhe Shang,Zhanyou Chi,Can Li,Ce Hao,Govindjee Govindjee,Yantao Shi
For natural oxygenic photosynthesis, there is a consensus that H 2 O is oxidized to molecular oxygen by photosystem II (PSII) in the grana, while CO 2 assimilation takes place, long after oxygen evolution, in light-independent reactions, for example, through the Calvin-Benson Cycle in the stroma. Here, we report, for the first time, light-driven CO 2 assimilation by the PSII core complex, where the formation of methanol, along with the oxygen evolution, is validated by in - situ mass spectrometry, gas chromatography and isotopic labeling experiments. Such an unusual CO 2 assimilation is likely to be a simultaneous event along with the usual electron transfer occurring in normal light–independent assimilation. This discovery is extraordinary and is of great significance as it may substantially modify our understanding of the mechanism of photosynthesis.
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 11
·3383-3391
·
IF 2.936
Zhang Luping,Tu Xuewei,Han Weihang,Chen Liangchen,Chen Yutong,Zheng Hui
As the main resource of greenhouse gas, CO 2 needs to be fixed into different chemicals to relieve the environmental problem. Fe-based catalyst and g-C 3 N 4 have received extensive attention due to their easy preparation, low cost, and environmental friendliness. Herein, a heterogeneous catalyst system consisting of rich-electron g-C 3 N 4 and strong electron-withdrawing groups Fe-complex [Fe(bpy)(CO) 2 (Cl) 2 ] was developed, which could promote electron transfer and enhance the electronic interaction for fixing CO 2 . o -phenylenediamine substrates with different electron-donating/withdrawing groups were employed to fix CO 2 into high-valued heterocycle benzimidazoles. The optimum reaction conditions were examined by orthogonal experiments. A series of benzimidazole derivatives were synthesized with yield up to 98%, which indicated the catalyst had the ability of fixing CO 2 . This catalyst provides a new pathway for fixing CO 2 into valuable benzimidazole derivatives. Graphical Abstract
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EcoMat
·
2023
·Vol. 5
·期 5
·e12334
·
IF 14.6
Juhee Jang,Shangqian Zhu,Ernest Pahuyo Delmo,Tiehuai Li,Qinglan Zhao,Yinuo Wang,Lili Zhang,Hongwen Huang,Jingjie Ge,Minhua Shao
Despite of superior performance of the oxide-derived copper (OD-Cu) in producing valuable hydrocarbons during CO 2 RR, its fabrication process is still ambiguous and complicated. In this work, we develop a simple microwave-assisted method to synthesize the oxide-derived Cu nanosheet (OD-Cu NS) and reveal that the oxidation state of Cu species is controlled by varying the Cu precursor amount. Notably, the simultaneous formation of nano-sized Cu domains influence the surface roughness of OD-Cu NS. The partially oxidized Cu surface exhibits a superior faradaic efficiency (FE) of C 2+ products up to 72%, along with a partial current density of 55 mA cm −2 in a neutral KHCO 3 solution. More importantly, the as-obtained OD-Cu NS shows a synergetic effect on dissociating of CO 2 molecules by the strong binding energy and promoting of C 2+ compounds productivity by the enlarged electrochemical surface area. This work provides a new insight for designing efficient OD-Cu catalysts toward CO 2 RR.
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Nature Catalysis
·
2022
·Vol. 6
·期 1
·6-15
·
IF 40.706
Kong Shuyi,Lv Ximeng,Wang Xin,Liu Zhengzheng,Li Zichuang,Jia Bingquan,Sun Du,Yang Chao,Liu Lijia,Guan Anxiang,Wang Jiacheng,Zheng Gengfeng,Huang Fuqiang
Methanol manufacturing by CO 2 electrolysis is a potential near-zero-emission route to carbon neutrality, but most of the previous studies in aqueous electrolytes have achieved poor methanol selectivity and yield. Inspired by hard–soft acid–base theory, we proposed that the CO 2 electroreduction pathways towards methanol or methane could be switched by tuning the electron delocalization state of Cu catalytic sites. On the basis of this hypothesis, we have designed and synthesized a cuprous cyanamide (Cu 2 NCN) crystal in which isolated Cu(I) ions strongly conjugated with NCN 2− exhibit highly delocalized electrons. Theoretical calculations showed that Cu 2 NCN substantially reduces the Cu–O interaction of the adsorbed *OCH 3 intermediate so that it is weaker than the O–C interaction at the critical reaction bifurcation point of Cu‒*O‒CH 3 , thus switching the pathway to release *OCH 3 and form methanol. The Cu 2 NCN catalyst exhibits one of the highest recorded CO 2 -to-CH 3 OH selectivities (70%) and an outstanding partial current density of −92.3 mA cm −2 in aqueous electrolyte, corresponding to a CH 3 OH electroproduction rate of 0.160 μmol s −1 cm −2 .
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CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Yi Sun,Wei Zhang,Shan Lu,Wenhua Miao,Meiling Chen,Fei Liu,Haining Na,Jin Zhu
Herein, a novel cellulose-based fluorescent material with amine-responsive property was developed in a CO 2 switchable solvent for the contactless, real-time, and visual monitoring of the freshness of shrimp , crab, and fish. A nucleophilic cellulose carbonate intermediate is in-situ formed upon dissolution of cellulose in the CO 2 switchable solvent, which is adopted for the highly effective grafting of poly( l -lactic acid) and amine-responsive fluorescent reagent 7-amino-4-(trifluoromethyl) coumarin onto the cellulose backbone via ring opening polymerization and nucleophilic substitution reaction, respectively. The product has good processibility, and sensitive and reversible fluorescent responsive towards ammonia. The fluorescent intensity of the material decreased significantly and its fluorescent color changed from blue to cyan, when the aquatic products got spoiled. This study indicates that the CO 2 switchable solvent has great potential for the modification of cellulose with various functionality by taking advantage of the highly active nucleophilic cellulose carbonate intermediate.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Zhizhou Cai,Ning Cao,Fanxing Zhang,Xiangzhou Lv,Ke Wang,Yi He,Yao Shi,Hao Bin Wu,Pengfei Xie
Electrocatalytic CO 2 reduction into ethanol driven by renewable energy represents a promising strategy for energy storage and mitigation of global warming, but it has remained challenging to gain high activity and selectivity of ethanol. Here we take advantage of atomic arrangement in immiscible Ag-Cu composite during annealing and establish hierarchical interfaces in the obtained core-shell catalyst. The atomic Ag-Cu interactions increase electrochemical surface area and expedite charge dynamics, resulting in an unprecedented electrocatalytic performance with the faradaic efficiency of C 2+ products, ethanol as 80.2 %, 52.6 % and the current density of ∼320 mA cm −2 at −1.0 V (versus reversible hydrogen electrode). Moreover, the Ag-Cu catalyst exhibits a notable stability for ∼60 h. Mechanism studies reveal that local CO intermediates preferentially accumulate on the core, then migrate to the continuous Cu surface for C-C coupling energy-favorably toward ethanol. Our work highlights a novel design principle as interface engineering for advanced tandem electrocatalysts.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Nan Li,Zhi Wang,Jixiao Wang
Carbonic anhydrase (CA)-inspired membranes for CO 2 separation were constructed by introducing hydroxypropyl-β-cyclodextrins (Hβ-CDs) into the polyamide networks, which were formed via interfacial polymerization reactions between trimesoyl chloride and tertiary amino-containing monomers . Hydrophobic inner cavities of Hβ-CDs with the hydrophilic exterior can be used to simulate the hydrophobic pockets of CA enzymes. Hydrophilic and hydrophobic regions were constructed via introducing Hβ-CDs into membranes, while the transport of nonpolar CO 2 molecules and polar components (H 2 O and HCO 3 − ) in CO 2 hydration reactions could be enhanced. Meanwhile, tertiary amino groups in biomimetic membranes can act as the base catalysts for CO 2 hydration reactions, which were deemed as carriers for facilitated transport membranes. Biomimetic membranes containing Hβ-CDs and tertiary amino groups exhibited outstanding CO 2 permeance of 2792 GPU and CO 2 /N 2 selectivity of 171 at 0.15 MPa, showing the potentials for low-pressure CO 2 capture. Particularly, CO 2 transport mechanisms were also analyzed for biomimetic facilitated-transport membranes, which can supply new visions for developing novel membrane materials for CO 2 separation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shudan Chi,Yi Ye,Xinglei Zhao,Junteng Liu,Junsu Jin,Le Du,Jianguo Mi
Greenhouse gases lead to frequent natural disasters, and CO 2 emissions from flue gases account for nearly half of anthropogenic CO 2 emissions. As an adsorbent, molecular sieves show excellent CO 2 adsorption; however, their defects limit their industrial application. To solve the problem of powder blockage and H 2 O absorption, we proposed the in-situ growth of molecular sieve in polyacrylate matrix beads to obtain molecular sieve composite for CO 2 capture in flue gas after combustion. Compared with those of pristine NaY, the CO 2 adsorption capacity of NaY@PA composite increased by 17.9 % and the H 2 O adsorption capacity decreased by 36.6 %. For further reduction in H 2 O absorption, post-modified composite NaY-ZIF@PA was synthesized by loading ZIF on NaY@PA surface to form a bilayer composite structure. The H 2 O absorption of NaY-ZIF@PA was reduced by 54.8 %, thus ensuring highly efficient CO 2 adsorption.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Yimeng Zhou,Qianjin Ye,Xiangli Shi,Qiong Zhang,Qi Song,Changjian Zhou,Di Li,Deli Jiang
Due to the multiple electron and proton transfer processes involved, the photogenerated charges are easily recombined during the photocatalytic reduction of CO2, making the generation of the eight-electron product CH4 kinetically more difficult. Herein, Ni3B nanoparticles modulated by p-block element were combined with TiO2 nanosheets to construct a novel Schottky junction photocatalyst (Ni3B/TiO2) for the selective photocatalytic conversion of CO2 to CH4. The formed Ni3B/TiO2 photocatalyst with Schottky junction ensures a transfer pathway of photogenerated electrons from TiO2 to Ni3B, which facilitates the accumulation of electrons on the surface of Ni3B and subsequently improves the activity of photocatalytic CO2 reduction to CH4. The optimized Ni3B/TiO2 Schottky junction shows an improved CH4 yield of 30.03 μmol g–1 h–1, which was much higher than those of TiO2 (1.62 μmol g–1 h–1), NiO/TiO2 (2.44 μmol g–1 h–1), and Ni/TiO2 (4.3 μmol g–1 h–1). This work demonstrated that the introduction of p-block elements can alleviate the scaling relationship effect of pure metal cocatalysts to a certain extent, and the modified Ni3B can be used as a promising new cocatalyst to effectively improve the selective photocatalytic of CO2 to CH4.
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