CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Di Zeng,Haipeng Wang,Xiaodi Zhu,Heng Cao,Yuanyi Zhou,Weimin Wang,Ling Zhang,Wenzhong Wang
Selective production of C 2+ chemicals from photocatalytic CO 2 reduction remains a big challenge due to the inert CO 2 molecular and vague C C coupling process. Herein, contributed by its uniform hexagonal pores, two-dimensional h'-H x WO 3 is selected as the support to realize single atom Cu loading (Cu/WO 3 ). Under the irradiation of light, the h'-H x WO 3 transformed into electron- and proton-rich tungsten bronze, which ensured the supply and transfer of multiple electrons/protons for the CO 2 reduction. Meanwhile, the similar coordination environment and appropriate distance of the Cu active sites presented by the Cu/WO 3 not only enable the adsorption and activation of CO 2 but also enhance the efficient C C coupling. Thus, Cu/WO 3 photocatalyst achieves the conversion of CO 2 to CH 3 COOH with a selectivity of 67 %, which is about 17 times higher than that of pristine h'-H x WO 3 . This work expands the route to prepare highly active single-atom catalysts, benefiting CO 2 photoreduction to selective reduction products.
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NEW CARBON MATERIALS
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2022
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IF 3.7
Hui-nian Zhang,Hui-qi Wang,Su-ping Jia,Qing Chang,Ning Li,Ying Li,Xiao-lin Shi,Zi-yuan Li,Sheng-liang Hu
Developing highly selective, economical and stable catalysts for the electrochemical conversion of CO 2 into value-added carbon products to mitigate both CO 2 emission and the energy crisis is challenging. We report an efficient and robust electrocatalyst for the CO 2 reduction reaction (CO 2 RR) by embedding CoN 4 active sites in a graphene matrix. These highly dispersed CoN 4 sites show an extraordinary CO 2 RR activity, with a high CO Faradaic efficiency of nearly 95% at −0.76 V (vs. RHE) and remarkable durability. The corresponding overpotential is 0.65 V. Our finding could pave the way for the design at the atomic scale of highly efficient electrocatalysts for the CO 2 RR.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2022
·Vol. 46
·期 12
·17015-17028
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IF 4.672
Xueliang Sun,Qilong Wang,Yuyu Liu,Jin Yi,Jiujun Zhang
Summary CO 2 reduction to produce value-added chemicals/fuels is generally considered as an effective way to solve the energy crisis and global warming. However, the greatest challenge to the technology is the lack of high-performance catalysts as this process is quite sluggish under mild conditions. Herein, we have carefully prepared a series of bimetallic Pb x Cd y nanoparticles (NPs) as well as their monometallic counterparts via a facile chemical reduction. Electrocatalytic performances of obtained catalysts were evaluated with respect to chemical composition, electrolytic potential, and so on. All of them exhibit high performance and achieve high faradaic efficiency for HCOOH production (FE HCOOH ) over a voltage window of −1.16 to −1.26 V vs the reversible hydrogen electrode (V RHE ). Among them, Pb 3 Cd 1 achieved a maximum FE HCOOH of 96% at −1.16 V RHE and a desirable stability over 12 hours of continuous electrolysis. The excellent performance of Pb 3 Cd 1 can be attributed to the huge specific area of NPs and the synergistic effect of the components. This study shows that efficient bimetallic Pb x Cd y electrocatalysts have a large application potential for highly selective HCOOH production from CO 2 . Highlights Bimetallic PbCd nanoparticles were synthesized by facile chemical reduction for electrocatalytic CO 2 reduction. PbCd nanocatalysts performed well in highly active, selective, and stable HCOOH electrosynthesis from aqueous CO 2 . Pb 3 Cd 1 achieved maximum HCOOH faradaic efficiency of 96% at −1.16 V RHE , a record as far as we know. A stable current density (>7 mA cm −2 ) can be kept after a 12-hours continuous electrolysis.
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Nano-Micro Letters
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2022
·Vol. 14
·期 1
·1-13
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IF 23.655
Li Xiaotong,Wang Jianghao,Lv Xiangzhou,Yang Yue,Xu Yifei,Liu Qian,Wu Hao Bin
Dual-site electrocatalysts with in situ formed metal-oxide interfaces are proposed and demonstrated to enhance the formation of multi-carbon products from electrochemical CO 2 reduction.
The 0.5-UiO/Cu delivers a high C2+ Faradaic efficiency of over 74% with notably boosted formation rate and durability, surpassing most reported electrocatalysts.
A unique mechanism of UiO-66 to induce in situ reconstruction of Cu surface and formation of UiO-66-derived amorphous ZrO x /Cu interface is uncovered, which improves the selectivity and productivity toward C2+ products.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2022
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IF 0.847
Wei Fu,Jiajie Fan,Quanjun Xiang
ABSTRACT The production of renewable fossil fuels such as CH 4 and CO by photocatalytic CO 2 reduction has attracted more and more attention. However, single photocatalyst is less efficient for photocatalytic reduction of CO 2 due to the fast recombination of photogenerated electron pairs. Herein, we successfully prepare CdS-Ag 2 S composite by assembling the Ag 2 S QDs cocatalyst on the surface of CdS nanosheet-assembled flower through oil-bath solvothermal method . This composite is prepared through a simple self-assembly strategy using cadmium chloride, ammonia and thiourea as precursors of the CdS nanosheet-assembled flower and silver nitrate and 3-mercaptopropionic acid as the precursors of Ag 2 S QDs. The average diameter of Ag 2 S QDs is apparently 6.0 nm. The light absorption edge of the composite is at around 560 nm, with the corresponding band gap at 2.14 eV. The CdS-Ag 2 S QDs composite with 5 wt% Ag 2 S QDs loaded achieves CO evolution rate of 16.6 μmol•g −1 •h −1 without noble-metal cocatalysts. This strengthened photocatalytic performance and photocatalytic stability were attributed to the energy band broadening of Ag 2 S QDs caused by quantum size effect and the large specific surface area due to the assembled flower. The mechanism underlying the enhanced photocatalytic CO 2 reduction activity is further proposed. This study demonstrates that semiconductor-based quantum dots are strong candidates for excellent cocatalysts in photocatalysis .
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Bingying Jia,Bang Xu,Liujie Bing,Jihong Sun,Shiyang Bai
With the assistance of cetyltrimethyl ammonium bromide (CTAB), the delamination of disorderly layered clinoptilolite (CP) was performed. The introduction of CTAB in hydrothermal system was beneficial to stratification of CP lamellas by enlarging interlayer spacing, and thus accelerating the formation of disordered CP nanosheets . The hydrophobic alkyl chain restricts the crystal growth along a-axis and the few-layer CP lamellas with integrally preserved heulandite structures were obtained by ultrasonic treatment and HNO 3 modification at room temperature. Meanwhile, the CTAB-assisted crystallization mechanism was further elucidated, in which, the amorphous spherical nanoparticles were firstly generated and then transformed into the fibrous and lamellar species. Finally, the flower-like CP morphologies with the aggregated nanosheets appeared. Meanwhile, the selective adsorptions and separations of CO 2 and CH 4 using these delaminated CPs as the absorbents were preliminarily explored, showing a strong potential in the mixed gases separation applications. This approach is a promising strategy for constructing delaminated zeolites with low n(SiO 2 /Al 2 O 3 ), which may open a new avenue for the delaminated CP nanosheet applications in gas adsorption and separation fields.
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Molecular Catalysis
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2022
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IF 5.089
Yifan Liu,Li Dong,Yichao Wang,Qian Su,Xianghai Meng,Weiguo Cheng
Polymeric ionic liquid membranes (PILMs) were prepared by photo-initiated polymerization of DMAEMA-based ionic liquids (ILs) and co-monomers for the conversion of CO 2 into cyclic carbonates. The influences of functional groups and anions were investigated to find the optimal ionic liquid monomer. The PILM based on [DMAEMA-EtOH]Br exhibited the highest propyl carbonate (PC) yield (98%), which was close to that of the [DMAEMA-EtOH]Br monomer. Moreover, the PILMs can catalyze the gas state propylene oxide (PO) and CO 2 into PC with a PO conversion of 87.3%, while the PO conversion of the pure polymeric ionic liquids was only 3.1% for gas state PO. The excellent catalytic activity can be attributed to the highly active catalytic sites and superb swelling ability of PILMs. The dry PILMs could absorb the PO vapor and swell into membranes with abundant pores, which contained plentiful active sites to catalyze PO and CO 2 to PC efficiently.
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ChemSusChem
·
2022
·Vol. 15
·期 19
·e202201386
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IF 9.14
Zhenzhen Zhou,Xiao Liu,Jian-Gong Ma,Peng Cheng
Graphical It's a trap ! Through a new “ligand-in-dimer-trap” strategy, the host–guest composites featuring metal–organic framework-encapsulated binuclear NHC−Co complex ( Co 2 @MOF) is prepared and used as a double-sites catalyst, which combines and surpasses the advantages of homo- and heterogeneous catalysis and exhibits prime performance in converting CO 2 into widely used formamides under ambient conditions. Environmental problem caused by carbon emission is of widespread concern. Involving CO 2 as C 1 resource into chemical synthesis is one of the most attractive ways for carbon recycling. Herein, the first example of host–guest composites featuring metal–organic framework (MOF)-encapsulated binuclear N-heterocyclic carbene (NHC) complex, Co 2 @MIL101, was developed with the molecularly dispersed [Co(IPr)Br] 2 (μ-Br) 2 ( Co 2 ) loading in the cage of MIL-101(Cr) via a “ligand-in-dimer-trap” strategy, which was comprehensively investigated through various techniques including synchrotron X-ray absorption, electron microscopy, X-ray diffraction, solid-state nuclear magnetic resonance spectroscopy, and others. The noble-metal-free double-sites catalyst Co 2 @MIL101 exhibited promising stability, activity, efficiency, reusability, and substrate adaptability for converting CO 2 into various formamides with amines and hydrosilanes and achieved the best performance for one of the most useful formamides, N -methyl- N -phenylformamide (MFA), among the recyclable catalysts at ambient conditions, providing a reliable approach to successfully unify the advantages of both homo- and heterogeneous catalysts. Density functional theory calculations were applied to illustrate the superior activity of the binuclear NHC complex center as double-sites catalyst toward the activation of CO 2 .
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GREEN CHEMISTRY
·
2022
·Vol. 24
·期 21
·8292-8301
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IF 11.034
Cong Luo,Jiayi Wang,Houfang Lu,Kejing Wu,Yingying Liu,Yingming Zhu,Binshen Wang,Bin Liang
An ideal strategy for the management of greenhouse gas carbon dioxide (CO2) and surplus industrial product-glycerol (Gly) is to convert them into the valuable glycerol carbonate (GC). However, conventional conversion processes rely on high CO2 pressure and reaction temperature. In this work, a series of easily prepared protic ionic liquids (ILs) were studied for the one-pot synthesis of GC using CO2, Gly, and styrene oxide (SO). A 94% yield of GC was obtained with the catalysis of 1,8-diazabicyclo[5.4.0]undec-7-enenium iodide (HDBUI) under atmospheric pressure at 45 °C. Experimental results and density functional theory (DFT) calculations suggest that the high catalytic activity of HDBUI is attributed to the strong nucleophilicity and substrate activation afforded by the synergistic effect of the protic HDBU+ cation and I− anion. In addition, high GC yields were also obtained when simulated flue gas and crude Gly were used as substrates.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Shangguan Wenchao,Liu Qing,Wang Ying,Sun Ning,Liu Yu,Zhao Rui,Li Yingxuan,Wang Chuanyi,Zhao Jincai
Achieving CO 2 reduction with H 2 O on metal photocatalysts and understanding the corresponding mechanisms at the molecular level are challenging. Herein, we report that quantum-sized Au nanoparticles can photocatalytically reduce CO 2 to CO with the help of H 2 O by electron-hole pairs mainly originating from interband transitions. Notably, the Au photocatalyst shows a CO production rate of 4.73 mmol g −1 h −1 (~100% selectivity), ~2.5 times the rate during CO 2 reduction with H 2 under the same experimental conditions, under low-intensity irradiation at 420 nm. Theoretical and experimental studies reveal that the increased activity is induced by surface Au–O species formed from H 2 O decomposition, which synchronously optimizes the rate-determining steps in the CO 2 reduction and H 2 O oxidation reactions, lowers the energy barriers for the *CO desorption and *OOH formation, and facilitates CO and O 2 production. Our findings provide an in-depth mechanistic understanding for designing active metal photocatalysts for efficient CO 2 reduction with H 2 O.
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ENERGY & FUELS
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2022
·
IF 4.654
Shumei Chen,Chao Miao,Lixing Liang,Jing Ouyang
This paper reports the synthesis and CO2 methanation performance of Ni/CeO2–ZrO2 (CZ) solid solutions assembled on different clay minerals (rectorite, attapulgite, halloysite, and kaolin). The catalytic performance of the samples was examined in temperature range 200−400 °C at normal pressures. The attapulgite (ATP) assembled Ni nps-incorporated-CZ solid solution (Ni–CZA) has the highest CO2 conversion and excellent stability. The CO2 conversion of the Ni–CZA catalyst reached up to 81.2% at 400 °C, and CH4 selectivity was nearly 100%. The catalyst assembled on ATP has excellent adsorption performance and a large specific surface area, resulting in higher Ce3+ and adsorbed oxygen content, thanks to the high content of oxygen vacancies and faster oxygen transfer speed. Mechanistic analysis shows that the H2 dissociates at the Ni site, the CO2 was decomposed into CO and O, and the ATP and CZ provide hydroxyls and oxygen vacancies, respectively, in this composite catalyst.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Yachen Deng,Shifu Wang,Yanqiang Huang,Xuning Li
MOF-based materials have been widely explored in electrochemical CO 2 reduction reactions for the production of valuable chemicals. Understanding the reconstruction of those catalysts under working conditions is crucial for the identification of active sites and clarification of reaction mechanism. Herein, a series of six N coordinated Sn-based metal-organic frameworks (Sn-N6-MOFs) are newly developed for electrochemical CO 2 reduction (CO 2 RR). 2% Sn-N6-MOF achieves the optimal catalytic performance with a formate Faradaic efficiency of ∼85% and a current density of 23 mA·cm −2 at −1.23 V vs. RHE. In-situ Raman results combined with ex-situ 119 Sn Mössbauer measurements reveal the structural reconstruction of Sn-N6-MOFs during CO 2 RR, generating tin nanoclusters as the real active sites for CO 2 electroreduction to HCOOH.
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