Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Zhou Min,Wang Zhiqing,Mei Aohan,Yang Zifan,Chen Wen,Ou Siyong,Wang Shengyao,Chen Keqiang,Reiss Peter,Qi Kun,Ma Jingyuan,Liu Yueli
The precise construction of photocatalysts with diatomic sites that simultaneously foster light absorption and catalytic activity is a formidable challenge, as both processes follow distinct pathways. Herein, an electrostatically driven self-assembly approach is used, where phenanthroline is used to synthesize bifunctional LaNi sites within covalent organic framework. The La and Ni site acts as optically and catalytically active center for photocarriers generation and highly selective CO 2 -to-CO reduction, respectively. Theory calculations and in-situ characterization reveal the directional charge transfer between La-Ni double-atomic sites, leading to decreased reaction energy barriers of *COOH intermediate and enhanced CO 2 -to-CO conversion. As a result, without any additional photosensitizers, a 15.2 times enhancement of the CO 2 reduction rate (605.8 μmol·g −1 ·h −1 ) over that of a benchmark covalent organic framework colloid (39.9 μmol·g −1 ·h −1 ) and improved CO selectivity (98.2%) are achieved. This work presents a potential strategy for integrating optically and catalytically active centers to enhance photocatalytic CO 2 reduction.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Wenjun Zhang,Jian Liu,Zhong Jin
The electrochemical system based on water, CO2, and electricity is the key technology to realize the coexistence and combination of renewable energy and fossil energy, which can convert CO2 molecules into high-value-added products under mild and controlled conditions, thus achieving carbon neutrality. Designing efficient electrocatalysts to realize highly active, selective, and stable CO2RR has become one of the vital issues. Particularly, the nanostructure design and interface adjustment of electrocatalysts have been regarded as the key points for improving their catalytic performance. Herein, a tin dioxide hollow nanotube (SnO2 HNT) catalyst with a three-dimensional cross-linked network structure has been fabricated by electrospinning and rapid-heating calcination. The morphology and component structure of SnO2 HNTs were analyzed by a series of characterizations. The performance in electrocatalytic carbon dioxide reduction reaction (eCO2RR) was further tested. Owing to the hollow nanostructure, the catalyst possessed a large specific surface area and abundant active sites, which greatly accelerated mass transport and electron mobility. During eCO2RR, SnO2 HNTs achieved a peak faraday efficiency value of 87.4% for C1 products at −1.1 V vs RHE, which significantly suppressed the occurrence of hydrogen evolution side reactions. In addition, compared with the commercial SnO2 nanoparticles or partially reduced Sn/SnO2, the catalytic activity and selectivity of CO2-to-formate conversion significantly increased under the same potential, indicating that the optimization of electronic/geometric structure for high-yield metal oxides can effectively improve the comprehensive performance of eCO2RR.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Jiachen Sun,Néstor Guijarro,Peihang Li,Udayabhaskararao Thumu,Jun-Ho Yum,Kevin Sivula,Zhiming M. Wang
One of the promising methods to solve the current energy and environment issues is photoelectrochemical (PEC) water splitting and CO2 reduction reaction. Chalcopyrite copper indium gallium sulfide (CIGS) and CuIn0.3Ga0.7S2 nanocrystal thin films have been considered photovoltaic materials, and here, we demonstrated their potential to reduce CO2 into CO. A modified solution process affords to decrease the number of surface ligands, which triggers an increase in the crystal size and an improved reproducibility in performance and output current. After depositing gold nanoparticles on the surface of CIGS, the Faradic efficiency related to the CO2-to-CO conversion can reach 12.93% in aqueous electrolytes and 25% in nonaqueous electrolytes. Further investigation points out that in the range of applied potential between −0.1 and −0.2 V vs a reversible hydrogen electrode (RHE), the CIGS photocathode appears to display a stable photocurrent density for 1 h, but when applying a higher applied bias, such as of −0.3 V vs RHE, the degradation of the current is significant. Additionally, we found that coupling catalysts to the CIGS increases the selectivity toward CO and minimizes the competitive hydrogen evolution reaction.
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Energy Technology
·
2023
·Vol. 11
·期 8
·2300119
·
IF 3.8
Shiyuan Liu,Ce Zhang,Wei Yao
Electrochemical CO 2 $\left(\text{CO}\right)_{2}$ reduction reaction is considered as a promising technical route for carbon-neutral and mitigating greenhouse effect. CO 2 $\left(\text{CO}\right)_{2}$ concentration limitation hinders the performance of state-of-the-art electrochemical CO 2 $\left(\text{CO}\right)_{2}$ reduction reaction. Increasing the mass transfer of reactants on the catalyst surface by flow cell design and porous electrode design has become the mainstream approach. Studying the distribution of mass in reaction region is important and beneficial to optimizing and designing efficient reactors. Herein, electrochemical CO 2 $\left(\text{CO}\right)_{2}$ reduction reaction reactors with micrometer and millimeter channels are simulated and systemically analyzed. The results reveal the microfluidic design can improve the mass transfer and reactant gas flow in the porous layer to reduce the concentration polarization and ensure uniform local potential of the reactor. A micrometer channel model requires only 10 sccm inlet gas supply to achieve the same current density compared to a millimeter flow channel with an inlet flow of 20 sccm. This study proposes a reasonable flow channel reactor to reduce gas stagnant region, which not only enhances the CO 2 $\left(\text{CO}\right)_{2}$ reduction performance effectively with evident potential dependence, but also guides the design for large-scale reactors.
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National Science Review
·
2023
·Vol. 11
·期 2
·
IF 20.6
Du Xiaowei,Zhang Peng,Zhang Gong,Gao Hui,Zhang Lili,Zhang Mengmeng,Wang Tuo,Gong Jinlong
Gas diffusion electrodes (GDEs) mediate the transport of reactants, products and electrons for the electrocatalytic CO2 reduction reaction (CO2RR) in membrane electrode assemblies. The random distribution of ionomer, added by the traditional physical mixing method, in the catalyst layer of GDEs affects the transport of ions and CO2. Such a phenomenon results in elevated cell voltage and decaying selectivity at high current densities. This paper describes a pre-confinement method to construct GDEs with homogeneously distributed ionomer, which enhances mass transfer locally at the active centers. The optimized GDE exhibited comparatively low cell voltages and high CO Faradaic efficiencies (FE > 90%) at a wide range of current densities. It can also operate stably for over 220 h with the cell voltage staying almost unchanged. This good performance can be preserved even with diluted CO2 feeds, which is essential for pursuing a high single-pass conversion rate. This study provides a new approach to building efficient mass transfer pathways for ions and reactants in GDEs to promote the electrocatalytic CO2RR for practical applications.
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CARBON
·
2023
·
IF 10.9
Ruijia Wang,Jianyong Wan,Hongda Guo,Bing Tian,Shujun Li,Jian Li,Shouxin Liu,Tony D. James,Zhijun Chen
Converting CO 2 with various epoxides to cyclic carbonates is extremely important. However, most of catalysts for such conversion either require complicated fabrication or are obtained from unsustainable sources. Motivated by this problem, we prepare biomass-based “all-in-one” carbon dots as nano-organocatalysts for firstly converting CO 2 to cyclic carbonates. In this work, carbon dots (CD@KI) with high catalytic performance and good recyclability are prepared from sodium phytate (SP), polyethylenimine (PEI) and KI using one-pot hydrothermal treatment featuring cheap precursors and simple operation. Assisted by highly catalytic activity of CD@KI, up to 99.5% yield is achieved for converting CO 2 and various epoxides to cyclic carbonates under mild conditions (solvent-free and 1 atm of CO 2 ). Moreover, the conversion yield is maintained for reactions up to 10 g in scale. Significantly, by taking advantage of the inherent luminescence of CD@KI, the as-formed cyclic carbonates catalysed by CD@KI can be directly converted to afterglow polymer composites .
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Ning Li,Chao Ma,Mao Ye,Xiangyu Guo,Zhihua Qiao,Chongli Zhong
Mixed-matrix membranes (MMMs) have arisen as an energy-saving and efficient candidate for CO 2 separation that can mitigate the greenhouse effect. However, challenges still remain in achieving good filler-polymer compatibility and high separation performance. Herein, a mechanochemistry method is proposed to synthesize an amine-functionalized ultramicroporous ZIF-62 (ZIF-UC-6) with good CO 2 affinity. Amino functional groups and open metal sites are introduced into ZIF-UC-6, which significantly improve its CO 2 adsorption capacity of ZIF-62. According to the ideal adsorption solution theory (IAST) calculation, the CO 2 /CH 4 and CO 2 /N 2 selectivity of ZIF-UC-6 is ∼80 and ∼140, respectively. Besides, when ZIF-UC-6 is incorporated into Pebax, hydrogen bonds can form between filler and polymer, which can increase the interfacial compatibility in the MMMs. The optimized membrane possesses a CO 2 permeability of ∼560 barrer, together with high CO 2 /CH 4 and CO 2 /N 2 selectivity of 41.8 and 86.2, surpassing the corresponding upper bounds. Moreover, the prepared MMMs have good pressure resistance and long-term stability. This work demonstrates an effective route for developing MMMs with good interfacial compatibility and high CO 2 separation performance for potential industrial applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Ruijie Chen,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic CO 2 reduction can simultaneously alleviate the energy crisis and solve environmental issues. Nevertheless, it is still challenging for designing photocatalysts with efficient carrier mobility in rational. Herein, the Bi 2 MoO 6 /g-C 3 N 4 (BMO/CN) heterostructure was constructed through a microwave-assisted which could enhance the construction of two-dimensional and two-dimensional (2D/2D) structures. The 2D/2D BMO/CN heterojunction possessed excellent charge separation efficiency which exhibited superior performance on photocatalytic CO 2 reduction. It was shown by the characterization that the (131) surface of Bi 2 MoO 6 was constructed with the (100) surface of g-C 3 N 4 . The work functions of Bi 2 MoO 6 and g-C 3 N 4 were determined to be 4.57 and 4.22 eV, respectively, which suggested the type-II heterojunction was formed. The formation of CO and CH 3 OH over the optimized BMO/CN-30% catalyst reached 2.44 and 3.61 µmol⋅g −1 ⋅h −1 , respectively. The immediate products of HCO 3 - were observed within in-situ FT-IR to further certify the evolution of CH 3 OH. This work highlighted a microwave-assisted strategy to build a heterojunction structure for enhancing photoreduction CO 2 .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yan-Fei Mu,Jin-Shuang Zhao,Li-Yuan Wu,Ke-Ying Tao,Zhao-Lei Liu,Fu-Quan Bai,Di-Chang Zhong,Min Zhang,Tong-Bu Lu
Strong photoresponse, efficient charge separation, and high surface activity are three important requirements for an ideal photocatalyst, while few photocatalysts can fully meet these requirements. Herein, we report such a photocatalyst based on lead-free halide perovskite hollow nanospheres (H-Cs 3 Sb 2 Br 9 ) by a facile antisolvent-assisted method. The hollow structure of H-Cs 3 Sb 2 Br 9 improves the light-harvesting performance; The formation of surface shallow trap states contributes to promoting the excited-carrier separation; The ligand-free termination surface of H-Cs 3 Sb 2 Br 9 facilitates the exposure of Br vacancies and active sites, thus strengthens the CO 2 adsorption and accelerates surface reactivity dynamics. As a result, with a dinuclear Co(II) complex as the co-catalyst, H-Cs 3 Sb 2 Br 9 exhibits a record-high photocatalytic activity for CO 2 reduction, with a CO yield of 15,010.4 ± 550.4 μmol g −1 after 8 h of illumination under simulated solar light (100 mW cm −2 ). This research presents a new way to develop cost-effective photocatalysts for CO 2 reduction.
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Journal of Environmental Sciences
·
2023
·
IF 6.9
Xiaoyun Chen,Guohua Jing,Bihong Lv,Zuoming Zhou
The non -aqueous solid-liquid biphasic solvent of 2-amino-2-methyl-1-propanol (AMP)/piperazine (PZ)/dipropylene glycol dimethyl ether (DME) features a high CO 2 absorption loading, favorable phase separation behavior and high regeneration efficiency. Different with the liquid-liquid phase change solvent, the reaction kinetics of CO 2 capture into solid-liquid biphasic solvent was rarely studied. In the present work, the reaction kinetics of CO 2 absorption into AMP/PZ/DME solid-liquid biphasic solvent was investigated into the double stirred kettle reactor. The absorption reaction followed a pseudo-first-order kinetic model according to the zwitterion mechanism. The overall reaction rate constant ( k ov ) and the enhancement factor ( E ) of CO 2 absorption both increased with increasing temperature. The total mass transfer resistance of the absorbent decreased with increasing temperature and increased with increasing absorption loading, so the higher reaction temperature was conducive to the absorption, and the liquid phase mass transfer resistance was the main factor affecting the absorption rate.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 33
·e54268
·
IF 3
Shoucun Zhang,Yujing Bian,Xueyin Yan,Guoli Fang,Shengwei Guo
The separation of the proteins is of great theoretical and practical importance for biotechnological application. Considering the requirement of non-destructive separation, the stimulus–response method is an alternative to the separation of protein. In this work, a cellulose-based composite with CO 2 stimulus–response property is prepared by a simple coprecipitation of poly ( N , N ˊ-diethylamino ethyl methacrylate)- co -poly (hydroxyethyl methacrylate) (PDH) and cellulose mixture solution. Subsequently, these composites as the adsorption medium are used to separate the bovine serum albumin (BSA, as the model protein) from solution through stimulus–response course (by CO 2 /N 2 alternation). The results indicate that the ratio of the copolymers/cellulose composite have an obvious effect on the separation of BSA. The average maximum adsorption capacity can get to 562.6 mg/g, and the composites exhibits good adsorption/desorption cycling characteristics. After the composite materials are cycled for three times, the adsorption capacity can still decrease to 300 mg/g. Due to its high adsorption capacity and low preparation cost, the composite is expected to be widely used in industry.
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Catalysts
·
2023
·Vol. 13
·期 7
·1030
·
IF 3.9
Siyi Jiang,Yujing Weng,Yangbin Ren,Shihang Meng,Xiaoman Li,Chao Huang,Yulong Zhang,Qi Sun
The chemical transformation of carbon dioxide (CO2) not only reduces the amount of carbon dioxide emitted into the Earth’s atmosphere by humans, but also produces carbon compounds that can be used as precursors for chemical and fuel production. Herein, a selective catalytic conversion of carbon dioxide to methanol is achieved by a bifunctional molybdenum disulfide catalyst (MoS2) with magnesium oxide and nickel and potassium promoters. Molybdenum disulfide prepared by the supercritical ethanol method has a large specific surface area and presents good catalytic performance with high methanol selectivity when loaded with potassium (K) and nickel (Ni) promoters. In addition, the catalysts were evaluated and it was founded that the addition of the K-promoter improved methanol selectivity. This research provides a new strategy for improved product selectivity and space–time yield (STY) of methanol in CO2hydrogenation.Keywords:CO2hydrogenation;molybdenum disulfide;methanol
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