Chemistry-An Asian Journal
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2024
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IF 3.5
Yicheng Wang,Qiyu Zhang,Chenxu Wang,Ayeza,Yating Zhang,Chao Hu
The utilization of renewable energy for electrocatalytic carbon dioxide reduction reaction (CO 2 RR) represents a pivotal technology in sustainable carbon conversion. Single-atom catalysts (SACs) featuring transition metal-nitrogen-carbon (M−N−C) structures have demonstrated exceptional electrocatalytic efficacy in CO 2 RR by maximizing atom efficiency. Nevertheless, further investigation is warranted to optimize the catalytic performance of SACs through the selection of suitable carbon sources and supports, as well as the modulation of the microenvironment surrounding individual metal atoms. In this study, a sulfur-doped Ni−N−C catalyst was prepared using a two-step strategy involving metal ion adsorption and thermal decomposition, with porous ion exchange resin serving as the carbon source. Due to the uniform distribution of single atom active centers on the resin-based carbon support and sulfur doping, this catalyst efficiently converts CO 2 into CO with a Faradaic efficiency exceeding 90 % within the range of −0.69~−1.29 V (vs. RHE), reaching a maximum value of 97.7 % (−0.79 V vs. RHE). Theoretical calculations indicate that second-shell sulfur doping effectively promotes coupled transfer of protons and electrons, leading to a significant reduction in Gibbs free energy barriers for CO 2 RR intermediate products.
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PubMed
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Journal of Materials Chemistry C
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2025
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IF 5.1
Shuang Xu,Lei Yang,Congya Wang,Liwei Pan,Jing Zhang,Yaling Wang,Hexiang Zhong
With the rapid development of industry, large-scale fossil energy consumption leads to the increase of atmospheric CO2 concentration and the resultant deteriorating global warming. The electrochemical reduction of CO2 (ERCO2) technology is a potential strategy to achieve the CO2 emissions reduction and to realize carbon recycling. However, the lack of high product selective, active and stable catalysts is one of the remaining challenges for the industrial applications of ERCO2. Herein, an electrochemical oxidation-reduction reconstruction method is developed to reconstruct the copper network without extra Cu salt addition obtaining Cu2O-Cu (111) catalysts with nanoporous structures for improving the selectivity and activity of CH4 and C2H4 product. The oxidation-reduction reconstruction derived catalyst achieves improved faradaic efficiency of 56.63% for CH4 product and a partial current density of 41.6 mA cm-2 at -1.38 V (vs. RHE). The selectivity and activity toward C2H4 are also improved. The catalytic superiority originates from synergistic interplay between the Cu₂O-Cu heterogeneous interface and high electrochemical active surface area. Additionally, the presence of abundant oxygen vacancies at the Cu2O-Cu interface accelerate the electron transfer process and promote the high selectivity and activity toward CO2-to-CH4. This study paves a new way for enhancing the selectivity and activity of CO2 electrocatalytic conversion to CH4.
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FUEL
·
2025
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IF 7.5
Zekai Miao,Hao Ge,Xinran Han,Rui Wu,Hai Zhu,Congchao Zhang,Shengping Wang
The coal gasification fine slag (FS) is a solid waste rich in Si components. The preparation of high-performance mesoporous silica for CO 2 capture using FS as raw materials will alleviate environmental pollution. The alkali-fusion method was used to obtain the high activated Si-containing precursor which could be completely dissolved in NaOH solution with low alkalinity concentration (3 %). The mesoporous silica with highly ordered hexagonal phase was prepared which had high surface area of 1629 m 2 /g and pore volume of 0.8 cm 3 /g. The Si concentration had the great effect on the yield of mesoporous silica and the mechanism for the formation and growth of mesoporous silica between high and low Si-precursor concentration was different. In the preparation process for high yield of mesoporous silica, the silicate ions primarily tended to adsorb around the cetyltrimethylammonium bromide micelles to form nuclei and then the silicate reacted preferentially with the surface silanol groups on the existing particles rather than generating new nuclei. The condensation of the silicate at the external surface of the surfactant micelles occurred to grow into large particles. However, the mesoporous silica particles formation in the lower concentration of silicate species in the alkali solutions was mainly contributed to the interactions between silicate species and CTAB rather than the deposition of silica species. The mesoporous silica showed high CO 2 adsorption performance. The breakthrough time of MS-8 occurred at 22 min and CO 2 adsorption capacity was 2.3 mmol/g at 25 °C. All these results suggest that the silica in fine slag could be fully utilized to prepare mesoporous silica which had a great potential to be used for practical and industrial CO 2 adsorption applications.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2024
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IF 4.8
Ying Gao,Jiafeng Zhang,Yanan Tu,Weidong Wang,Ziqi Zhu,Zhiqiang Xu
The preparation of hierarchical porous silica aerogels from coal gasification fine slag (CGFS) offers an effective approach to achieving high-value utilization of solid waste and reducing the production cost of solid adsorbent matrix materials. However, the main challenges involve overcoming technical barriers to efficiently and value-added conversion of CGFS into silica aerogels with CO₂ adsorption properties, as well as elucidating the phase transformation mechanisms during the synthesis process. In this study, CGFS was used as the raw material to obtain a silicon-containing precursor through pre-decarbonization (with ash content as high as 99.82 %) and alkali dissolution treatment. A hierarchical porous silica aerogel was then synthesized using an efficient hydrothermal process. The effect of alkali dissolution on silicon extraction and the phase transformation mechanisms were thoroughly discussed, and the leaching mechanism was analyzed through thermodynamic and kinetic models. The results showed that the high leaching rate of silicon was attributed to the presence of a large amount of amorphous SiO₂ in the decarbonized fine slag (DCFS), while the formation of zeolite Na-P1 and hydroxysodalite during the alkali dissolution process affected the efficiency of silicon extraction. Then, the structural formation mechanism and CO₂ adsorption properties of the hierarchical porous silica aerogels were analyzed using N₂ adsorption-desorption and CO₂-TPD. The SiO₂-1-30-0.5 exhibited a high CO₂ adsorption ability of 1.53 mmol g −1 , and the CO₂ adsorption capacity maintained 94.78 % of the original value and after 5 adsorption-desorption cycles.
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Nature Communications
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2024
·Vol. 15
·期 1
·1-10
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IF 14.7
Deng Huiying,Liu Tingting,Zhao Wenshan,Wang Jundong,Zhang Yuesheng,Zhang Shuzhen,Yang Yu,Yang Chao,Teng Wenzhi,Chen Zhuo,Zheng Gengfeng,Li Fengwang,Su Yaqiong,Hui Jingshu,Wang Yuhang
CO 2 electroreduction is a potential pathway to achieve net-zero emissions in the chemical industry. Yet, CO 2 loss, resulting from (bi)carbonate formation, renders the process energy-intensive. Acidic environments can address the issue but at the expense of compromised product Faradaic efficiencies (FEs), particularly for multi-carbon (C 2+ ) products, as rapid diffusion and migration of protons (H + ) favors competing H 2 and CO production. Here, we present a strategy of tuning the 2-position substituent length on benzimidazole (BIM)-based copper (Cu) coordination polymer (CuCP) precatalyst – to enhance CO 2 reduction to C 2+ products in acidic environments. Lengthening the substituent from H to nonyl enhances H + diffusion retardation and decreases Cu-Cu coordination numbers (CNs), favoring further reduction of CO. This leads to a nearly 24× enhancement of selectivity towards CO hydrogenation and C-C coupling at 60 mA cm −2 . We report the highest C 2+ product FE of more than 70% at 260 mA cm −2 on pentyl-CuCP and demonstrate a CO 2 -to-C 2+ single-pass conversion (SPC) of ~54% at 180 mA cm −2 using pentyl-CuCP in zero-gap electrolyzers.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Peng Zhang,Cai Liang,Mudi Wu,Yongjie Li,Xiaoping Chen,Daoyin Liu,Jiliang Ma
The efficiency and sustainability for the recycling of plastic wastes into hydrogen was investigated. An integrated microwave-driven valorization of plastic wastes and CO 2 for H 2 and CO production was proposed. Specifically, plastic wastes were decomposed into H 2 and solid carbons, followed by carbon elimination via CO 2 gasification under microwave irradiation. Through the high-throughput screen of catalysts as well as the optimization of key parameters, over 96% hydrogen was converted into H 2 with a yield of 480 mmol∙g −1 H plastic while the carbon conversion and CO 2 conversion reached up to 70% and 53%. The five-cycle successive test displayed extraordinarily high and stable catalytic activity due to the facile elimination of carbon deposition. The application for real-world plastic wastes further demonstrated the efficient microwave-driven CO 2 gasification of plastic wastes into H 2 and CO production as a feasible and sustainable technology toward the waste-to-energy circular economy.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Zicheng Yang,Yuming Xie,Yi Feng,Jianfeng Yao
The effective utilization of biomass resources can bring significantly environmental and economic benefits. In this context, tea saponin, which can be easily and extensively extracted from the oil cake as the biomass waste during the seed oil production from camellia seeds, is explored as the precursor to synthesize porous carbon bearing abundant –OH and –COOH groups via a simple carbonization process. Owing to the obtained porous structure and existence of rich oxygen-containing groups serving as Lewis acidic sites, the carbonized tea saponin (CTS) can display impressive catalytic activities for CO 2 cycloaddition reaction with both high selectivity (> 99%) and high yield of target cyclic carbonate under either thermally driven (80 °C and 0.1 MPa CO 2 ) or photo-thermally driven (UV-Vis light irradiation with the light intensity of 350 mW/cm 2 ) conditions. In addition, benefiting from the good chemical stability, CTS can be reused for many cycles with almost no catalytic activity loss, making CTS a promising biomass-based catalyst for CO 2 fixation under mild conditions.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Sensen Zhou,Yueli Wen,Bin Wang,Maohong Fan,Lu Ren,Zheng Cui,Wei Huang,Jing Li,Jianping Guo
CO 2 hydrogenation to C 2+ OH is an effective way to diminish CO 2 emissions. Although challenges still exist in large-scale applications, CuFeZn catalysts attract extensive attention due to their low-cost. Herein, CuFeZn catalysts are modified by different amounts of K 3 PO 4 , (KP) 0.1 CuFeZn exhibits an excellent catalytic performance (total alcohols selectivity of 15.76 % at CO 2 conversion of 38.10 %, C 2+ OH/ROH fraction of 94.23 %, and C 2+ alcohols space–time-yield (STY) of 53.81 mg·mL −1 ·h −1 ). Combined with a series of characterization results, it is found that the effect of K 3 PO 4 is complex, and the proportion of Fe 2+ , Cu 0 and medium base shows perfect linear relation to STY of C 2+ OH. The significance level of the above three factors is in the following sequence: Cu 0 ＞Fe 2+ ＞medium base. The introduction of K 3 PO 4 decreases the proportion of Fe 2+ (active site for RWGS, the competitive reaction for C–C coupling) and increases the proportion of Cu + /(Cu + +Cu 0 ) (Cu + is the active site for C–C coupling) due to the synergistic effect of Cu 0 and Cu + , thereby improving the synthesis of C 2+ OH. Moreover, conversion of Fe 0 to Fe 3 C or Fe 3 O 4 plays negative roles in the stability of the catalysts.
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JOURNAL OF POWER SOURCES
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2025
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IF 7.9
Minglu Wang,Yun Da,Meiqiu Xie,Zheng Wang
Solid oxide electrolysis cell (SOEC) is recognized as a promising and efficient energy conversion technology by converting CO 2 into CO for achieving carbon neutrality. However, the cathode materials with insufficient electrocatalytic activity and stability greatly limit its large-scale commercial application. Herein, a synergistic strategy of high-entropy engineering and anion doping is proposed to develop a novel highly efficient and stable cathode material for CO 2 electrolysis in SOEC. Fluorine doped high-entropy perovskite La 0.6 Sr 0.4 Fe 0.3 Co 0.2 Ni 0.2 Mn 0.2 Mo 0.1 O 3-δ (LSFCNMM-F) is successfully synthesized to boost the CO 2 electrolysis performance. F doping can weaken the strength of metal-oxygen bond, increasing the concentration of oxygen vacancies, which significantly promotes the CO 2 adsorption and activation. Accordingly, F-doped high-entropy perovskite LSFCNMM-F cathode exhibits outstanding electrochemical performance and excellent stability for CO 2 electrolysis in SOEC. Compared to the pure high-entropy perovskite LSFCNMM, F-doped high-entropy perovskite LSFCNMM-F achieves 24.5 % improvement in current density with a remarkable value of 1.78 A/cm 2 at 1.5 V and 800 °C, surpassing most of the reported cathode materials in SOEC field. Moreover, the single cell with LSFCNMM-F cathode exhibits better long-term stability than that with pure high-entropy perovskite LSFCNMM cathode during 100 h operation at 1.2 V and 750 °C, owing to the inhabitation of Sr segregation on the electrode surface after F doping. The results from this study provide insights into the role of synergistic strategy for combining high-entropy engineering and anion doping in developing highly efficient and stable cathode for CO 2 electrolysis using SOEC technology.
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ACS Catalysis
·
2024
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IF 11.3
Shuo Cao,Zun Guan,Ying Ma,Bing Xu,Jun Ma,Wei Chu,Riguang Zhang,Giuliano Giambastiani,Yuefeng Liu
The design and synthesis of highly efficient and selective catalysts for CO2 thermal reduction remain a challenging issue of modern catalysis. Molybdenum carbide has attracted great interest in CO2-to-CO conversion (Reverse Water Gas Shift process, RWGS) because of its ability to dissociate CO2 and H2. However, single dominant Mo- or C-terminated facets of molybdenum carbide are unlikely to activate CO2 and H2 molecules simultaneously. Herein, we demonstrate how structural diversity of cogenerated molybdenum species (i.e., Mon nanoclusters and Mo2C nanoparticles) on the surface of an oxygen-enriched C-carrier boosts synergistically the chemoselective RWGS process with rates up to 581 μmolCO2·gMo–1·s–1 with CO selectivity > 99% already at 400 °C under an H2-rich environment. This catalytic outcome ranks among the highest reported so far for molybdenum carbide- or noble metal-based catalysts in the process, and it is up to 1.8 times higher than that measured on Mo2C-based nanoparticles. The enhanced reactivity of the structurally mixed catalyst has been ascribed to a synergistic modulation of the geometrical and electronic structure of different Mo sites that reduces the temperature at which CO production starts and facilitates the chemoselective CO desorption pathway. Experimental and in silico studies have also unveiled the existence of a linear correlation between the percentage of high-valence molybdenum species in the metal active-phase composition (Moδ+ %) and the increase in the RWGS rate.
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Molecular Catalysis
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2024
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IF 3.9
Zhenzhen Wang,Encheng Liu,Zhonghua Sun,Zhihui Zhang,Mingyang He,Qun Chen,Junfeng Qian
Formic acid (FA) is of great significance given its extensive applications in various industrial fields. At present, methanol carbonylation is the main industrial production process of FA. However, this process uses two kinds of raw materials from fossil fuels and emits a large amount of CO 2 . Alternatively, converting CO 2 into FA can not only achieve the production of value-added chemicals but also effectively address environmental issues caused by CO 2 emission. To improve the low reactivity of CO 2 , homogeneous and heterogeneous catalytic systems have been widely evaluated, among which heterogeneous catalytic systems are attracting ever-increasing attention owing to their great industrialization prospects. However, some of these heterogeneous catalysts suffer from low catalytic performance. Herein, PdAu alloy nanoparticles anchored on amine-functionalized hierarchical porous carbon (PdAu/HPC-AP) were constructed to drive efficient converting of CO 2 into FA. Characterization and testing results demonstrated that the introduced Au atoms caused lattice distortion and charge redistribution on the surface of the bimetallic catalyst, facilitating the adsorption and activation of reaction molecules. Furthermore, the modification of HPC with an appropriate amount of amine ligands was found important to the chemical adsorption of CO 2 and the dispersion of PdAu NPs. The Pd 60 Au 40 /HPC-AP catalyst with the optimum synergy of alloy and ligand demonstrated excellent activity for the target reaction with a TOF value of 486 h –1 at 100 °C. Moreover, it can even catalyze the reaction at room temperature with a TOF value of 13 h –1 .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Xiaole Dong,Shihui Wang,Bingqi Tan,Xiangyi Geng,Futang Liu,Penghao Gao,Peiling Gao,Jiutao An,Xinpeng Liu,Qingmei Meng
Different nanoparticles were introduced into the N-ethylethanolamine/diethylaminoethanol/p-Xylene biphasic absorbent to form nanofluid systems, and the CO 2 capture performance was investigated. The CO 2 capture performance of the absorbent was significantly enhanced by introducing 0.1 wt% CuO nanoparticles, with a first absorption carbon capacity of 0.09952 g CO 2 ·g −1 absorbent. In the first cycle of regeneration, [email protected] % CuO nanofluid had a carbon capacity of 0.07654 g CO 2 ·g −1 absorbent, achieving an efficiency improvement of 35.73 %. Its regeneration energy consumption was reduced by 0.3256 GJ·t -1 CO 2 , representing a 15 % decrease compared with the base liquid. The cyclic absorption capacity was enhanced significantly after the addition of CuO, with a CO 2 capacity at 0.0690 g CO 2 ·g -1 absorbent after four cycles. The characterization of CuO revealed the stability of nanoparticles in nanofluids. In addition, it was found that the nanoparticles exhibited phase-transfer characteristics. After absorption, they accumulated in the rich phase and then became uniformly distributed throughout the entire liquid phase following regeneration. This behaviour could promote a more efficient desorption process. This study provides a new approach for green chemistry and carbon capture applications.
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