NEW JOURNAL OF CHEMISTRY
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2025
·
IF 2.5
Zhile Xiong,Yuewen Chen,Weidong Xie,Jiali Huang,Xiaoli Zhang,Xiya Zhang,Hai Liu
The electrocatalytic reduction of CO2 using renewable electricity offers a sustainable approach for the production of valuable chemicals. However, this process is often hindered by low catalytic activity and poor selectivity. In this study, we have developed a novel electrocatalyst that integrates ZIF-8-regulated ZnO interfaces, undercoordinated surface sites, and mesoporous nanostructures. This design enabled the ZnO/ZIF-8 catalyst to achieve excellent CO2 conversion performance, with a CO2 Faraday efficiency of more than 91% over the potential range of -1.0 V to -1.6 V and a high current density compared to reversible hydrogen electrodes. At the optimal potential of -1.4 V, the CO Faraday efficiency reaches 95.57%, accompanied by a current density of -8.16 mA/cm2. The porous nature and superior CO2 adsorption ability of the ZIF-8 shell layer foster an optimal setting for CO2 conversion while enhancing the exposure of active sites. Additionally, the synergistic coupling of ZnO and ZIF-8 interfaces fine-tunes the electronic structure of the active sites, thereby enhancing CO2RR efficiency.
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NEW JOURNAL OF CHEMISTRY
·
2025
·Vol. 49
·期 18
·7384-7392
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IF 2.5
Zhaolin Xu,Xiaolong Yang,Senmiao Liu,Bo Wang,Yanhua Peng,Yan Zhang,Zhuo Li
In this study, three preparation methods were used to modify MCM-41 to enhance the CO2 adsorption capability. That is, grafting, impregnation and a two-step method combining the grafting and impregnation. It was demonstrated that amine grafting and subsequent impregnation of MCM-41 significantly enhanced the CO2 adsorption capacity than single amine alone. The maximum adsorption capacity of 5.49 mmol g−1 was obtained on MCM-41 with 1% 3-aminopropyltriethoxysilane (APTES) grafting and subsequent 60% triethylenetetramine (TETA) impregnation (named as M-1AP-60TETA), which also showed good adsorption cycling stability for ten cycles. This was attributed to the synergistic effect of APTES and TETA, where the formation of an intertwined network enhanced CO2 diffusion and carbamate formation.
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Journal of Cleaner Production
·
2024
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IF 9.7
Menglei Mao,Ruqing Chong,Feixue Sun,Rui Gao,Zihui Meng,Xinlong Fan,Wenfang Liu
Enzymatic conversion of CO 2 to formate is a highly significant pathway for CO 2 utilization, but current level of conversion efficiency remains unsatisfactory due to low solubility of CO 2 under mild conditions. CO 2 -philic materials can significantly augment the reaction by raising local concentration of substrate. Herein, the intercalated Ti 3 C 2 T x , nano-silica (SiO 2 ) and carbon nitride (CN) with abundant CO 2 adsorption sites were introduced to fabricate Ti 3 C 2 T x based nanocomposites, Ti 3 C 2 T x /SiO 2 /CN (TSCN), for the first time. As the controls, binary composites including Ti 3 C 2 T x /SiO 2 (TS), Ti 3 C 2 T x /CN (TCN) and SiO 2 /CN (SCN) were also studied. For each kind of material, the composition, structure, morphology, and application performance in the enzymatic CO 2 conversion were characterized and influencing factors were investigated. Among these composites, TSCN exhibited the best application performance and the enzyme reaction was accelerated up to 23.9 times that of the blank system. The value could reach as high as 35.3 after polyethyleneimine (PEI) modification. Following that, PEI modified composites were used as carrier of formate dehydrogenase (FDH) and apparent specific activity was up to 2.8 times that of free enzyme, which could retain 88.2% of the initial value after 10 cycles associated with the structural integrity. This work provides new impetus to CO 2 capture and conversion in a clean and mild way that shows bright application prospects.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Zhicheng Zhang,Wei Zou,Hong Wang,Zhongjie Du,Chen Zhang
A high-performance biomass-based adsorption materials could be the promising trend for CO 2 capture and storage technology. However, the direct application of biomass-based porous materials as a CO 2 adsorbent with enhanced performance is an emerging issue. Herein, a facile synthesis and a biomimetic strategy were combined to prepare amine-functionalized chitosan foam for CO 2 capture, and then a porous biomass is achieved for the application on the environment protection field. Firstly, the chitosan foam was synthesized by the emulsion-templating method at room temperature. Depended on stabilizing n-octane in the chitosan hydrogel with Span 80, a tunable three-dimensional network porous structure was obtained. Subsequently, co -deposition with dopamine (DA) and polyethyleneimine (PEI) was applied to load abundant amine content on the surface of chitosan foam and thereby improving CO 2 adsorption capacity. Finally, the as-prepared amine-functionalized chitosan foam exhibited the impressive adsorption capacity of 3.59 mmol/g at 333 K and atmospheric pressure, and the better adsorption selectivity and stability. The results extend the preparation approach of biomass porous materials, and also its application in CO 2 adsorption technology.
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PubMed
高影响因子
Frontiers in Bioengineering and Biotechnology
·
2021
·
IF 5.89
Yang Ruigang,Zhu Lingyun,Li Tao,Zhu Lv-yun,Ye Zi,Zhang Dongyi
Metabolic engineering of cyanobacteria has received much attention as a sustainable strategy to convert CO2 to various longer carbon chain fuels. Pinene has become increasingly attractive since pinene dimers contain high volumetric energy and have been proposed to act as potential aircraft fuels. However, cyanobacteria cannot directly convert geranyl pyrophosphate into pinene due to the lack of endogenous pinene synthase. Herein, we integrated the gene encoding Abies grandis pinene synthase into the model cyanobacterium Synechococcus sp. PCC 7002 through homologous recombination. The genetically modified cyanobacteria achieved a pinene titer of 1.525 ± 0.l45 mg L−1 in the lab-scale tube photobioreactor with CO2 aeration. Specifically, the results showed a mixture of α- and β-pinene (∼33:67 ratio). The ratio of β-pinene in the product was significantly increased compared with that previously reported in the engineered Escherichia coli. Furthermore, we investigated the photoautotrophic growth performances of Synechococcus overlaid with different concentrations of dodecane. The work demonstrates that the engineered Synechococcus is a suitable potential platform for β-pinene production.
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PubMed
高影响因子
JOURNAL OF POLYMER RESEARCH
·
2025
·Vol. 32
·期 12
·467
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IF 2.8
Li Xiaoyun,Wang Zhen,Wang Junwei,Zhang Yingan,Kang Maoqing,Li Qifeng,Zhao Yuhua,Li Huanting
Bifunctional reactive cyclic carbonate compounds were synthesized and introduced into the epoxy system acting as diluting plasticizer and toughening agent to improve their plasticity and flexibility. Effects of content and structure of cyclic carbonates on the processibility, mechanical performances and thermal properties of the materials were investigated. An impressive improvement in viscosity reduction and mechanical performances is observed by loading of cyclic carbonate. The modified epoxy resin composites exhibit a significant enhancement in mechanical properties at a 30 wt% loading of cyclic carbonate with the tensile strength 170.6% higher than the original resin and 23.9% improvement in the flexural strength. The enhancement in material performance can be attributed to a combination of factors: the presence of soft segments, hydrogen bonding interactions, decrease in crosslinking density, and the plasticizing effect of unreacted components. Moreover, the thermal properties like degradation temperature, T g temperature and thermo-mechanical properties of epoxy resin composites were also affected by the introduction of cyclic carbonate.
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ENERGY & FUELS
·
2025
·
IF 5.3
Yuxia Zhu,Yuze Zu,Wei Xu,Yinghui Sun,Ying Li,Jie Bai
Coal gangue, the primary solid waste generated during coal mining, is mainly composed of silicon and aluminum oxide. Achieving its high-value utilization is crucial for resource recycling and sustainable development. In this study, we developed a method to synthesize ZSM-5 zeolite (ZSM-5-CG) using coal gangue as the sole silica–alumina source. The synthesis process, crystal growth mechanism, and catalytic performance of the resulting zeolites were systematically investigated. Compared with ZSM-5 prepared from commercial raw materials (ZSM-5-C), the coal gangue-derived synthesis required a significantly lower amount of template due to the favorable interaction between gangue-derived species and the template. Although crystallization in both systems follows the “solid–liquid phase transformation” mechanism, coal gangue, as a natural mineral source, exhibits significant differences in Si and Al coordination environment compared to commercial inorganic raw materials. These differences alter the dissolution and migration behaviors of Si and Al species in the mother liquor, leading to a synchronous release of these components during crystallization. As a result, nucleation and crystal growth processes happen more slowly, yielding a lower overall growth rate than that observed in systems derived from commercial raw materials. The obtained ZSM-5-CG was further applied in CO2 cycloaddition and methanation reactions, exhibiting catalytic activity comparable to that of ZSM-5-C, owing to its abundance of acid sites and large surface area. A cost analysis revealed that the total production cost of ZSM-5-CG was 29.7% lower than that of ZSM-5-C. This work provides a novel and economically viable route for the high-value utilization of coal gangue and highlights the potential of ZSM-5-CG in CO2 catalytic conversion.
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Nature Communications
·
2025
·
IF 15.7
Yu Yaodong,Wang Zuochao,Wang Weizhou,Han Jiani,Dong Tian,Jin Guangzhe,Li Hongdong,Lv Qingliang,Kutchin Alexander V.,Lai Jianping,Wang Lei
The development of efficient acidic CO 2 reduction reaction (CO 2 RR) to high value-added chemical HCOOH at high current density (>1 A cm -2 ) is crucial. However, addressing high potential, low Faradaic efficiency (FE), and poor stability simultaneously under acidic conditions remains challenging. Here, we construct small PdC x interstitial compounds and engineer the interstitial atoms to modulate the catalyst’s soft acid strength, thereby overcoming the triple challenge of “low overpotential-high current density-high stability” in acidic CO₂RR to HCOOH. Density functional theory (DFT) calculations and experimental characterization reveal that interstitial carbon infusion modulates Pd’s soft acid strength and weakens the Pd-O bond energy to form and desorb HCOOH, circumventing CO poisoning of the catalyst. Meanwhile, interstitial carbon infusion optimizes electronic structures, enhancing OCHO intermediate coverage as well as the effective retention and utilization of *H. This effect suppresses hydrogen evolution reaction (HER) while enhancing HCOOH selectivity. The optimized PdC 0.13 /CNT achieves >95% FE HCOOH and demonstrates stability in a proton exchange membrane (PEM) electrolyzer, maintaining 1000 mA cm -2 operation for 500 hours at 1.8 V cell voltage.
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ACS Nano
·
2021
·
IF 15.881
Zhiyi Wu,Chaoran Li,Zhao Li,Kai Feng,Mujin Cai,Dake Zhang,Shenghua Wang,Mingyu Chu,Chengcheng Zhang,Jiahui Shen,Zheng Huang,Yanling Xiao,Geoffrey A. Ozin,Xiaohong Zhang,Le He
The conversion of CO2 into fuels and feedstock chemicals via photothermal catalysis holds promise for efficient solar energy utilization to tackle the global energy shortage and climate change. Despite recent advances, it is of emerging interest to explore promising materials with excellent photothermal properties to boost the performance of photothermal CO2 catalysis. Here, we report the discovery of MXene materials as superior photothermal supports for metal nanoparticles. As a proof-of-concept study, we demonstrate that Nb2C and Ti3C2, two typical MXene materials, can enhance the photothermal effect and thus boost the photothermal catalytic activity of Ni nanoparticles. A record CO2 conversion rate of 8.50 mol·gNi–1·h–1 is achieved for Nb2C-nanosheet-supported Ni nanoparticles under intense illumination. Our study bridges the gap between photothermal MXene materials and photothermal CO2 catalysis toward more efficient solar-to-chemical energy conversions and stimulates the interest in MXene-supported metal nanoparticles for other heterogeneous catalytic reactions, particularly driven by sunlight.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Bowen Lu,Ziqiang Han,Xinyu Zhi,Liqi Zhang
NiFe 2 O 4 exhibits excellent redox properties and is widely applied in catalytic reactions. However, rapid inactivation under reaction conditions limited its industrial applications. In this study, CeO 2 -NiFe 2 O 4 composite catalysts were synthesized, and the Reverse Water Gas Shift (RWGS) reaction was measured to reveal its CO 2 hydrogenation performance under a high-temperature condition. NiFe 2 O 4 catalysts got deactivated after being reduced to Fe-Ni alloy at 700 °C, decreasing the CO 2 conversion rate. CeO 2 addition can significantly improve its high-temperature activity, and 20CeO 2 -NiFe 2 O 4 exhibited the best catalytic activity (80.85 %, 700 °C). The CeO 2 -confined maintained Ni-Fe alloy with a relatively small crystal size and larger specific surface area, supporting more active sites for CO 2 hydrogenation. CeO 2 addition induced higher oxygen vacancy concentration, enhancing CO 2 activation and formates species formed on 20CeO 2 -NiFe 2 O 4 , resulting in higher CO 2 conversion activity. In addition, 20CeO 2 -NiFe 2 O 4 maintained its catalytic stability for 50 h at 700 °C. The CeO 2 confined enhanced the high-temperature stability of Fe-Ni alloy. CeO 2 and formed CeFeO 3 dispersed in 20CeO 2 -NiFe 2 O 4 inhibited excessive aggregation of Fe-Ni alloy, and CeO 2 inhibited carbon deposition on Fe-Ni alloy, improving Fe-Ni alloy’s reaction stability under RWGS reaction conditions. CeO 2 confined may give insight into improving metal stability under high-temperature and reductive conditions in heterogeneous catalysis.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-9
·
IF 14.919
Liang Chu,Chen Yun,Wu Min,Wang Kai,Zhang Wenkui,Gan Yongping,Huang Hui,Chen Jian,Xia Yang,Zhang Jun,Zheng Shiyou,Pan Hongge
Environmentally benign synthesis of graphite at low temperatures is a great challenge in the absence of transition metal catalysts. Herein, we report a green and efficient approach of synthesizing graphite from carbon dioxide at ultralow temperatures in the absence of transition metal catalysts. Carbon dioxide is converted into graphite submicroflakes in the seconds timescale via reacting with lithium aluminum hydride as the mixture of carbon dioxide and lithium aluminum hydride is heated to as low as 126 °C. Gas pressure-dependent kinetic barriers for synthesizing graphite is demonstrated to be the major reason for our synthesis of graphite without the graphitization process of amorphous carbon. When serving as lithium storage materials, graphite submicroflakes exhibit excellent rate capability and cycling performance with a reversible capacity of ~320 mAh g –1 after 1500 cycles at 1.0 A g –1 . This study provides an avenue to synthesize graphite from greenhouse gases at low temperatures.
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RARE METALS
·
2024
·Vol. 43
·期 4
·1513-1523
·
IF 9.6
Zhang Ze-Yu,Wang Hai-Bin,Zhang Fei-Fei,Li Jing-Wei,Hu Xin-Zhuo,Yan Si-Wei,Bai Yi-Ming,Zhang Xun,Shen Gu-Rong,Yin Peng-Fei,Yang Jing,Dong Cun-Ku,Mao Jing,Liu Hui,Du Xi-Wen
Electrocatalysis of CO 2 reduction reaction is an effective way to convert CO 2 into high value-added products, but the selectivity of Cu-based catalysts for C 2+ products needs to be improved due to the high energy barrier of C–C coupling. Therefore, a viable catalyst design strategy to decrease energy barrier of C–C coupling should be put forward. Here, a nanocavity-enriched CuPd single atom alloy (CuPd SAA) catalyst is designed to promote C–C coupling process. The faradaic efficiency of CuPd SAA for ethylene and C 2+ reaches 75.6% and 85.7% at − 0.7 V versus reversible hydrogen electrode (RHE), respectively. Based on the results given by in situ characterization, the porous hollow structure dramatically increases the ratio of the linear-bond *CO, thus enhancing the faradaic efficiency for ethylene. Density functional theory (DFT) calculation reveals that the Pd doping can regulate the electronic structure of neighboring Cu atoms to decrease the energy barrier of C–C coupling, further improving the faradaic efficiency. This work provides a new idea for designing catalyst with high selectivity for ethylene. Graphical abstract
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