CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 39
·期 2
·246-252
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IF 2.726
Wang Renquan,Li Tiantian,Gao Rui,Qin Jiaqi,Li Mengyao,Guo Yizheng,Song Yujiang
With the excessive consumption of fossil fuels and the massive emission of CO 2 , it has led to a series of environmental crises posing a serious threat to sustainable development. Electrochemical CO 2 reduction reaction (CO 2 RR) to ethylene helps solve these serious environmental crises. Herein, we report the synthesis of a copper-based electrocatalyst by pyrolysis of yolk-shell structured HKUST-1 with partial substitution of trimesic acid by benzimidazole(nitrogen source). The electrocatalyst exhibits an ethylene Faradic efficiency(FE) of 25.8% and a partial ethylene current density of 23.7 mA/cm 2 , in addition, the electrocatalyst can maintain stable performance during 10 h of electrolysis, which are all better than those of the electrocatalyst without nitrogen dopant. According to electrochemical measurements and X-ray photoelectron spectroscopy(XPS), we propose that the nitrogen dopant plays an effective role in stabilizing Cu(I) species and promoting CO 2 molecules activation, as well as suppressing the reduction of Cu(I) species during electrolysis. Eventually, the performance of the electrocatalyst toward CO 2 RR is studied in a flow cell. This work provides a new route for the design of Cu-based electrocatalyst toward electrochemical CO 2 conversion into ethylene.
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ChemNanoMat
·
2022
·Vol. 8
·期 10
·e202200269
·
IF 3.82
Ziye Guo,Huanhuan Yang,Qingyong Tian,Wenjie Ma,Qun Xu,Buxing Han
Graphical A template- and surfactant-free top-down strategy was developed to transform non-vdW bulk CeO 2 into 2D amorphous CeO 2− x nanosheets with defective structure for the first time by cleaving Ce−O covalent bonds with the assistance of supercritical CO 2 . The unique nanosheets show outstanding UV-vis adsorption and photoluminescence properties due to the disordered atomic structure and increased vacancy defects (F-centers). Two-dimensional (2D) non-van der Waals (non-vdW) amorphous nanomaterials have attracted much attention for optical, catalytic and biomedical applications owing to their rich dangling bonds and unsaturated coordination. CeO 2 , a typical non-vdW material, with amorphous 2D structure and intrinsic optical properties have rarely been prepared via a top-down method due to the lack of anisotropy in its 3D bonding network. Herein, we develop an environmentally-friendly top-down method to achieve ultrathin 2D amorphous CeO 2− x with controllable defects from bulk CeO 2 by utilizing supercritical CO 2 . The unique CeO 2− x nanosheets exhibit outstanding ultraviolet-visible adsorption and photoluminescence (PL) properties due to the disordered atomic structure and increased vacancy defects resulting from the cleavage of Ce−O covalent bonds and amorphization of CeO 2 . In addition, the defect-related emission mechanism of the visible PL for the as-prepared 2D CeO 2− x nanosheets has been proposed.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
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2022
·Vol. 101
·期 2
·657-670
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IF 2.5
Yu Zhang,Jing Cai,Xiao-Sen Li,Zhao-Yang Chen,Gang Li
To investigate the effect of the particle size of porous media on CO 2 hydrate formation, the formation experiments of CO 2 hydrate in porous media with three particle sizes were performed. Three kinds of porous media with mean particle diameters of 2.30 μm (clay level), 5.54 μm (silty sand level), and 229.90 μm (fine sand level) were used in the experiments. In the experiments, the formation temperature range was 277.15–281.15 K and the initial formation pressure range was 3.4–4.8 MPa. The final gas consumption increases with the increase in the initial pressure and the decrease in the formation temperature. The hydrate formation at the initial formation pressure of 4.8 MPa in 229.90 μm porous media is much slower than that at the lower formation pressure and displays multistage. In the experiments with different formation temperatures, the gas consumption rate at the temperature of 279.15 K is the lowest. In 2.30 and 5.54 μm porous media, the hydrate formation rates are similar and faster than those in 229.90 μm porous media. The particle size of the porous media does not affect the final gas consumption. The gas consumption rate per mol of water and the final water conversion increase with the decrease in the water content. The induction time in 5.54 μm porous media is longer than that in 2.30 and 229.90 μm porous media, and the presence of NaCl significantly increases the induction time and decreases the final conversion of water to hydrate.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Ma Wenjing,Dai Shanshan,Li Xiaojiang,Hongsheng Lu
Oily wastes are easily generated in many processes of exploitation, solvent extraction is the common method for treating the oily waste. However, traditional solvent extractions are difficult to recycle the solvent, and oil is difficult to separated. As a low-volatility solvent, ionic liquid is simple in synthesis, low in cost, so it has good application prospect. In this work, the sustainable separation of oil from oily waste was implemented by using CO 2 -switchable ionic liquids. On the basis of solvent extraction, ionic liquids can reduced losses and costs. The CO 2 -switchable ionic liquids were prepared by poly (propylene glycol) bis(2-aminopropyl ether) D-230 and fatty acids with low volatility at the mole ratio of 1:2. Upon the alternate bubbling CO 2 and N 2, ionic liquids could be transformed alternately from water-miscible state to water-immiscible state. The water-immiscible state was bi-phasic system containing hydrophobic fatty acids and ammonium bicarbonate solution by bubbling CO 2 . Based on the bi-phasic system, the oil (kerosene, paraffin oil and crude oil) could be mixed with fatty acids, and were separated from fatty acids in the hydrophilic state upon N 2 , where the recovery rate of oil was more than 97% and fatty acids was not residual in recovered oil. Treating oily waste, the oil could be extracted from oily waste by the bi-phasic system. The ionic liquids were reused and the oil was separated by bubbling N 2 without extra additives, where the recovery rate of oil from oily waste was more than 85.57%. Due to the simplified process and negligible solvent loss, the economic benefit of recovering per barrel crude oil reached 76.7% of the price of crude oil. Compared with the existing technology , this sustainable separation is simpler, more economical and more environmentally friendly. Hence, it is expected that this sustainable separation based on CO 2 -switchable ionic liquids will meet the development of green separation with low-energy consumption.
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CHEMISTRY-A EUROPEAN JOURNAL
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2022
·Vol. 28
·期 55
·e202201430
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IF 5.02
Yuanyuan Zhang,Jian Liu
Graphical An artificial photosystem was constructed through the covalent attachment of Rh complex onto PCN. The integrated photocatalyst could regenerate NADH efficiently by integrating the light harvesting unit and the electron transfer unit through conjugated connection. By further coupling with FDH immobilized on the hydrophobic membrane, an enhanced HCOOH production could be obtained. Natural photosynthesis is a highly unified biocatalytic system, which coupled cofactor (NAD(P)H) regeneration and enzymatic CO 2 reduction efficiently for solar energy conversion. Mimicking nature, a novel system with Rh complex covalently grafted onto NH 2 -functionalized polymeric carbon nitride (NH 2 -PCN) was constructed. The integrated connection of the light-harvesting and electron mediation modules as Rh m3 -N-PCN could promote the efficient NAD + reduction to NADH. As a result, the integrated system exhibited a conversion of ∼66 % within 20 minutes. By further coupling in situ generated NADH with formate dehydrogenase (FDH), a photoenzymatic production of formic acid (HCOOH) from CO 2 was accomplished. Moreover, by immobilizing FDH onto a hydrophobic membrane, an enhanced HCOOH production of ∼5.0 mM can be obtained due to the concentrated CO 2 on the gas-liquid-solid three-phase interface. Our work herein provides an integrated strategy for coupling the anchored electron mediator with immobilized enzyme for enhanced artificial photosynthesis.
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Nano-Micro Letters
·
2022
·Vol. 14
·期 1
·1-16
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IF 23.655
Qiu Chen,Qian Kun,Yu Jun,Sun Mingzi,Cao Shoufu,Gao Jinqiang,Yu Rongxing,Fang Lingzhe,Yao Youwei,Lu Xiaoqing,Li Tao,Huang Bolong,Yang Shihe
For electrochemical CO 2 reduction to HCOOH, an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density ( J HCOOH ) at a low overpotential. Indium oxide is good HCOOH production catalyst but with low conductivity. In this work, we report a unique corn design of In 2 O 3- x @C nanocatalyst, wherein In 2 O 3- x nanocube as the fine grains dispersed uniformly on the carbon nanorod cob, resulting in the enhanced conductivity. Excellent performance is achieved with 84% Faradaic efficiency (FE) and 11 mA cm −2 J HCOOH at a low potential of − 0.4 V versus RHE. At the current density of 100 mA cm −2 , the applied potential remained stable for more than 120 h with the FE above 90%. Density functional theory calculations reveal that the abundant oxygen vacancy in In 2 O 3- x has exposed more In 3+ sites with activated electroactivity, which facilitates the formation of HCOO* intermediate. Operando X-ray absorption spectroscopy also confirms In 3+ as the active site and the key intermediate of HCOO* during the process of CO 2 reduction to HCOOH.
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Small
·
2022
·Vol. 19
·期 13
·2201305
·
IF 15.153
Boyu Yang,Shubin Li,Wei Mu,Zhao Wang,Xiaojun Han
The bottom-up constructed artificial cells help to understand the cell working mechanism and provide the evolution clues for organisms. The energy supply and metabolism mimicry are the key issues in the field of artificial cells. Herein, an artificial cell containing cyanobacteria capable of light harvesting and carbon dioxide fixation is demonstrated to produce glucose molecules by converting light energy into chemical energy. Two downstream “metabolic” pathways starting from glucose molecules are investigated. One involves enzyme cascade reaction to produce H 2 O 2 (assisted by glucose oxidase) first, followed by converting Amplex red to resorufin (assisted by horseradish peroxidase). The other pathway is more biologically relevant. Glucose molecules are dehydrogenated to transfer hydrogens to nicotinamide adenine dinucleotide (NAD + ) for the production of nicotinamide adenine dinucleotide hydride (NADH) molecules in the presence of glucose dehydrogenase. Further, NADH molecules are oxidized into NAD + by pyruvate catalyzed by lactate dehydrogenase, meanwhile, lactate is obtained. Therefore, the cascade cycling of NADH/NAD + is built. The artificial cells built here pave the way for investigating more complicated energy-supplied metabolism inside artificial cells.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 20
·7950-7956
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IF 4.569
Liuyong Chen,Jun Yang,Wenqian Yang,Jiahui Xian,Guangqin Li
Photochemical CO2 conversion into carbon fuel is a promising route to explore renewable energy and relieve climate change. However, it is still a key challenge to achieve high selectivity to CO and simultaneously achieve high conversion efficiency in photochemical CO2 reduction. Herein, we demonstrate the effect of Ni metal centers as catalytic active sites for the photocatalytic conversion of CO2 to CO by designing and constructing Ni metal–organic framework (Ni-MOF) materials. In pure CO2, Ni-MOF catalyst exhibits outstanding performance for visible-light-driven reductive CO2 deoxygenation with a high CO evolution rate of 19.13 μmol h−1 (per 1 mg of catalyst) and CO selectivity of 91.4%, which exceeds those of most reported systems. Upon using isostructural Co-MOF as the catalyst to replace Ni-MOF, a moderate performance towards CO2 photoreduction and low CO selectivity (40.1%) were observed, implying that the performance of CO2 photoreduction and CO selectivity are dependent on unsaturated metal centers.
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JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Xinyi Wan,Kuiyuan Zhang,Ting Wan,Youguo Yan,Zhizhen Ye,Xinsheng Peng
The emergence of Newton's cradle is promising for fast substance transport, which attracts tremendous attentions for industrial applications. Herein, an ultrafast and highly selective nano Newton's cradle for CO 2 transport is constructed through the assembly of negatively charged graphene oxide (GO) nanosheets and positively charged zinc hydroxide nanostrands (ZHNs), followed with impregnation of ionic liquid (IL) within the nanochannels. The GO laminates provide robust structure for whole system. The incorporation of IL endows the membrane with sieving ability to different gases while ZHNs play a key role to accelerate selective CO 2 adsorption, thus achieving exceptional CO 2 separation performance. The resulted nano Newton's cradle demonstrates that a huge CO 2 permeance enhancement of more than 53 times as that of the GO/IL membrane without ZHNs, superhigh CO 2 /light gases selectivities (35 for CO 2 /H 2 , 194 for CO 2 /CH 4 and 331 for CO 2 /N 2 ), out-stripping the Robeson upper bound of traditional polymeric membranes , as well as long-term operation stability. This innovative strategy not only provides an outstanding candidate for carbon capture, but also opens a new avenue to design separation membranes with high performance for various applications.
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Materials Advances
·
2022
·Vol. 3
·期 12
·4964-4972
·
IF 0
Chong Wang,Chengdeng Wang,Zhihao Xiong,Jiashuai Wang,Wenyuan Zhang,Haofeng Shi,Donghua Wang,Yousong Gu,Zhiming Bai,Yan Gao,Xiaoqin Yan
Electrochemical CO2 reduction reactions (CO2RRs) have been recognized as a promising solution to environmental and energy problems due to their ability to convert intermittent renewable electricity into hydrocarbon fuels and value-added chemicals. Copper has a unique ability to electrochemically reduce CO2 to produce C2+ hydrocarbon products compared to other metals. However, it is still suffering from low Faraday efficiency (FE) limitations for specific products. Herein, we have prepared an Ag-modified Cu/CuO–Ag catalyst with a porous structure via a galvanic replacement reaction method, which reduced CO2 to C2+ products with the FE of 52.5% at −1.1 V (vs. RHE). The experimental results and density functional theory (DFT) calculations show that the addition of Ag in Cu is beneficial to increasing the coverage of *CO on the Cu surface, which can decrease the potential barrier energy of the C–C coupling reaction and favor the generation of C2+ products. The results of this study may be helpful to the design of efficient tandem catalysts for electrochemical CO2 reduction.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Cong Liu,Qibin Zhu,Zhonghui Zhu,Chen Sun,Yimin Xuan,Kai Zhang
Foreigner element doping is one of effective strategies to promote photocatalytic reaction. Herein, a convenient one-step solvothermal method is applied to enable the isomorphic substitution of In 3+ in In(OH) 3 by Bi 3+ . The composition and microstructure of the photocatalysts were mainly obtained by X-ray diffraction (XRD), scanning electron microscope (SEM) and transmission electron microscope (TEM). UV–Vis diffuse reflectance and photoluminescence (PL) spectroscopy revealed the optical properties of photocatalysts. The surface properties of photocatalysts were mainly characterized by X-ray photoelectron spectroscopy (XPS). Theoretical calculations were used to reveal the reaction mechanism. The results indicated that CO production rate and selectivity of Bi 3+ doped In(OH) 3 are much higher than that of the pure In(OH) 3 , which could be attributed to the extended solar spectral response, the enhanced CO 2 adsorption capacity and the accelerated photogenerated carriers separation. The current work verifies the potential application of isomorphic substitution as an efficient route for solar fuel production.
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Sustainable Materials and Technologies
·
2022
·
IF 10.681
Boshu Jiang,Qiming Sun,Bachirou Guene Lougou,Hao Zhang,Xian Li,Zhibin Qu,Yong Shuai,Chi-Hwa Wang
The solar-driven thermochemical CO 2 conversion is an effective way to achieve the mission of carbon peaking and carbon neutrality . However, finding a material with excellent thermal stability, oxygen exchange capacity, and CO selectivity is one of the most important challenges in the thermochemical CO 2 conversion approach. This study investigated the solar thermochemical CO 2 -splitting characteristics through the synergistic thermal catalytic activity of CuO and NiFe 2 O 4 and the effect of SiC photothermal properties. The thermochemical redox cycling performance of CO 2 conversion through thermally activated catalysts was experimentally investigated via thermogravimetric combined quantum chemical calculations to provide comprehensive insights into the physicochemical principles underlying the thermochemical catalytic CO 2 -splitting. The X-ray diffraction, scanning electron microscopy, and energy spectrum detector technics were developed to gain detail on the crystal structure, surface morphology , and chemical composition changes in the reacting media. The newly synthesized composite material consisting of 25%CuO and 75%NiFe 2 O 4 (CNF-13) coated SiC porous skeleton resulted in higher CO 2 -splitting catalytic activity with an instantaneous CO production of 10.98mL ⋅ min ‐1 g CNF‐13 −1 and direct CO 2 -to-CO conversion rate of 33.9% at 1000–1200 K reaction temperature. The thermochemical CO 2 -splitting activity and redox stability of CNF-13@SiC was promoted by the photothermal properties of SiC support and the formation of Cu 2 O and Fe 3 O 4 new active material phases easing CO 2 reduction at low energy. This study provided experimental and theoretical findings that can be used as guidance for the fundamental research and application of CO 2 catalytic conversion into fuels through a solar thermochemical driven strategy.
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