INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Chunying Liu,Li Lv,Kun Liu,Junsu Jin,Jianguo Mi,Yongqiang Ren,Shisen Xu
By coupling CALF-20 on ZIF-7 via in situ crystallization in the confined micrometer-sized pores of poly(acrylates), a novel composite, namely, CALF-20-on-ZIF-7@poly(acrylates), has been synthesized for the simultaneous removal of CO2 and H2S from IGCC feed gas. Within this coupled crystal, CALF-20, known for its strong adsorption capacity and excellent stability toward CO2 and H2S, serves as the outer layer crystal to shift the adsorption/desorption hysteresis loop of inner ZIF-7 to beyond atmosphere pressure. Under high pressure, CO2 and H2S are automatically adsorbed. Upon reducing the pressure to the atmospheric level, CO2 is automatically released, while H2S remains temporarily due to its high adsorption energy. After about 150 cycles of CO2 adsorption/desorption of the kilogram-scale composite, H2S approaches saturation and is then removed by vacuuming. Since the content of H2S in IGCC feed gas is trivial, the total energy consumption for the composite regeneration is 0.16 MJ/kg (CO2). After 600 consecutive cycles, the CO2 adsorption capability of the composite decreases by 0.41%, demonstrating excellent cyclic stability.
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高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Xin Xie,Guilian Li,Shuo Geng
Bismuth oxide, a promising electrocatalyst for the formate production via electrocatalytic carbon dioxide reduction reaction (eCO 2 RR), suffers from structural instability at high overpotentials due to reduction-induced deactivation. This study proposes an innovative yttrium (Y) doping strategy that stabilizes Bi 2 O 3 through Y-Bi orbital interactions, effectively suppressing cathodic reduction during eCO 2 RR. Remarkably, the optimized 3 % Y-doped Bi 2 O 3 catalyst delivers outstanding performance, achieving a record formate Faraday efficiency (FE) of 97.9 % at −1.05 V vs. reversible hydrogen electrode (RHE) and maintaining FE > 90 % over a 350 mV potential window. Notably, it sustains FE exceeding 90 % even at industrial-grade current densities up to −160 mA cm −2 in flow cell configuration. Through systematic in situ spectroscopic characterization, density functional theory (DFT) calculations, and electrochemical analysis, we reveal that Y doping modulates the Bi−O electronegativity difference, which simultaneously stabilizes the Bi 3+ oxidation state and enhances adsorption of the critical *OCHO intermediate. This dual-function mechanism establishes a new paradigm for designing stable metal oxide electrocatalysts toward efficient formate electrosynthesis.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Mingrui Wang,Guanghui Zhang,Jie Zhu,Wenhui Li,Jianyang Wang,Kai Bian,Yi Liu,Fanshu Ding,Chunshan Song,Xinwen Guo
Unraveling the correlation between the structure of the active sites and the reaction pathway is of utmost importance to designing selective catalysts for efficient conversion of greenhouse gas CO 2 . In this contribution, the tunable selectivity of CO 2 hydrogenation to CO or CH 4 is achieved in response to the regulation of valance state of active cobalt species. We combined multiple in situ spectroscopic characterizations to show that the small CoO particles highly dispersed in the mesopores and interacted with SBA-15 support prefer to keep the oxidized state (+2). These CoO species is stable in bulk and the surface is partially reduced under the reactive conditions. More CoO sites exposed in this catalyst lead to the higher performance of reverse water gas shift reaction, whereas more metallic cobalt sites derived from the large CoO particles on regular SiO 2 mainly promote CO 2 methanation. In situ FT-IR experiments demonstrated that adsorbed formate dominates on CoO and serves as the key intermediate for the formation of CO, while the adsorbed carboxylate intermediate observed on Co 0 site is dissociated into adsorbed CO and then further hydrogenated to CH 4 . Stronger CO and H 2 adsorption and activation on Co 0 sites lead to the high CH 4 selectivity, whereas weakly bonded CO prefers to desorb from CoO site, resulting in the high CO selectivity. This work discloses the tunable selectivity and offers an opportunity for rational design of efficient cobalt catalysts aiming for selective CO 2 hydrogenation.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Li Fei,Zheng Wanjun,Jin Liequn,Cao Huazhen
Overusing fossil energy sources has led to global warming, seriously risking the habitability of the environments on which people depend. Photoelectrocatalytic (PEC) reduction of carbon dioxide (CO2) is a promising strategy to reduce CO2 into high-value-added chemicals and fuel products. However, photoelectrocatalysis faces problems related to low CO2 conversion efficiency and uncontrollable product complexity. This study reports a CuO–MoO3/TiO2NTs composite photoelectrode prepared by pulsed electrodeposition for the photoelectrocatalytic (PEC) reduction of CO2 to ethanol in a 1 M NaHCO3 medium under visible light irradiation and at an applied potential of −0.3 V vs. SCE. Molybdenum trioxide plays a regulatory role in the structure and properties of the photoelectrode. Photoluminescence analysis suggests that this occurs by introducing new energy levels between those of CuO and TiO2, which reduces the bandgap energy from 1.42 eV to 1.17 eV, promotes electron–hole pair separation, and significantly boosts photoelectrocatalytic activity. In addition, experimental results show that the doping of MoO3 enhanced the adsorption strength of the intermediate products and promoted the C–C coupling process. The optimized composite photoelectrode achieves 89% Faraday efficiency for ethanol at −0.5 V versus SCE (saturated calomel electrode). No new phases were generated during the catalytic process, confirming the stability of the CuO–MoO3/TiO2NTs composite photoelectrode.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Zicheng Yang,Jiale Ni,Yuming Xie,Yi Feng,Jianfeng Yao
The design presented here involves zeolitic imidazolate framework (ZIF) nanotubes wrapped with a mesoporous polydopamine (mPDA) layer to merge the structural and textural merits of both materials for efficient CO 2 fixation at room temperature under solvent-free and light irradiation conditions. The resulting tubular Zn-ZIF@mPDA composite (ZZ@mPDA) demonstrates significantly improved catalytic activity in CO 2 cycloaddition with epichlorohydrin, achieving a selectivity of > 99 % and a high yield of 96.9 % at 18 h, which is superior to that of pristine Zn-ZIF, with a yield of only 51.4 %. In addition, the mPDA layer confers good structural and chemical stability to ZZ@mPDA, resulting in negligible catalytic activity loss after five cycles. A mechanistic study indicates that the superior catalytic performance of ZZ@mPDA can be attributed to the combined photothermal and photocatalytic effects, involving the participation of both Lewis acidic/basic sites and photo-induced electron/hole pairs in the activation of CO 2 and epoxides. This research demonstrates the potential of ZIF@mPDA for photo-driven CO 2 conversion to cyclic carbonates and offers insights into the underlying mechanism.
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高影响因子
Industrial Chemistry & Materials
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2025
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IF 11.9
Xuehua Zhang,Chunlei Su,Rui Shi,Mingming Li,Lili Fu,Rongji Liu,Yong Chen,Bin Li,Guangjin Zhang
To enhance the charge separation efficiency of g-C3N4 and facilitate electron transfer between photosensitizer and molecular catalyst, polarization and coordination strategies are taken by grafting pyridine rings onto the edge of g-C3N4 framework. Herein, electron-withdrawing pyridine edge-functionalized g-C3N4 (g-C3N4-Px) was synthesized via a facile one-step thermal polymerization of urea and 4-aminopyridine, and employed as visible-light photosensitizer hybridized with cobalt phthalocyanine (CoPc) for efficient photoreduction of CO2. Both experimental and theoretical results confirm that electron-withdrawing pyridine grafting facilitates in-plane charge separation and directs electron migration toward the edge of g-C3N4, narrows its band gap for enhanced visible-light absorption, and provides dynamic coordination sites that significantly boost interfacial electron transfer from g-C3N4-Px to CoPc. A significant enhancement in CO yield was achieved with the optimized CoPc/g-C3N4-P1.5 hybrid, reaching 14.95 mmol g⁻¹ after 6 hours of visible-light irradiation—a 6.1-fold improvement over the unmodified CoPc/g-C3N4 (2.47 mmol g-1). This work paves a facile approach for developing highly efficient hybrid photocatalysts for CO2 reduction and improving the charge separation and visible light absorption in organic semiconductors.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Houde She,Yanan Qiao,Bin Liu,Shiyou Li,Lei Wang,Jingwei Huang,Qizhao Wang
The rising levels of atmospheric CO 2 caused by industrial activities have led to escalating global climate challenges, calling for efficient and sustainable carbon mitigation strategies. However, conventional graphitic carbon nitride (g-C 3 N 4 )-based systems are hindered by low charge separation efficiency, limited visible-light absorption, and poor CH 4 selectivity, significantly restricting their catalytic performance. In this study, a novel photothermal catalyst‑ruthenium nanoparticle-loaded and boron-doped multilayered C 3 N 4 nanosheets (4Ru-3B-C 3 N 4 )-was synthesized via supramolecular self-assembly, NaBH 4 -assisted impregnation, and thermal calcination. The structure, composition, and optoelectronic characteristics were systematically characterized through XRD, FTIR, SEM/TEM, XPS, UV–vis DRS, PL, EIS, and in situ DRIFTS, while the reaction mechanism and electronic structure were confirmed using density functional theory (DFT) calculations and work function simulations. Compared to pristine C 3 N 4 , the multilayered nanosheet architecture, B-doping, and anchoring of Ru nanoparticles synergistically facilitate the provision of active sites and promote the separation of photogenerated charge carriers. Furthermore, combined with density functional theory (DFT) calculations, we demonstrate that the Ru nanoparticles serve as active centers, endowing the catalyst with enhanced CO 2 adsorption and activation capabilities, while lowering the overall reaction energy barrier for the conversion of CO 2 to CH 4 . Under photothermal CO 2 reduction conditions, 4Ru-3B-C 3 N 4 delivers a high CH 4 production rate of 266.6 μmol·g −1 ·h −1 , which is approximately 24 times that of pristine C 3 N 4 . The anchored Ru nanoparticles also contribute to the excellent cycling stability exhibited by the designed photocatalyst. This active surface engineering strategy provides a new perspective for developing high-performance catalysts for CO 2 photothermal reduction.
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高影响因子
AICHE JOURNAL
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2025
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IF 4
Mengjiao Zhang,Tianbao Shi,Yitong Li,Bin Liu,Zhiwu Liang,Paitoon Tontiwachwuthikul,Jin-Heng Li
Amine-based chemical absorption remains a promisingly powerful technology for carbon dioxide (CO 2 ) capture. However, enhancing the performance of absorbents remains a significant challenge. In this study, three sterically hindered amines (SHAs), including 2-( tert -butylamino)ethanol, 2-amino-2-methyl-1-propanol, 2-amino-2-methylpropane-1,3-diol were selected as the primary absorbents with piperazine (PZ) employed as an activator. Absorption and desorption experiments were conducted for various PZ-SHAs systems with a total amine concentration of 30 wt% under conditions of 313 K and 13 kPa CO 2 partial pressure. The CO 2 absorption capacity, initial absorption rate, desorption rate, and desorption energy consumption were systematically evaluated, indicating that the addition of PZ as an activator could effectively improve the trapping capacity of the spatially hindered amine, and keep a high recycling capacity and low regeneration energy. Finally, the CO 2 reaction mechanism under the new system was clarified by 13 C nuclear magnetic resonance (NMR) technique.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Hui Ning,Rui Zhou,Minjun Zhou,Hongbin Wang,Yapeng Lv,Jiwei Wang,Dewen Song,Mingwang Wang,Dan Lu,Gaiyan Jiao,Xiaoli Ma,Xiaoshan Wang,Yanan Chen,Wenting Wu,Mingbo Wu
Carbon dioxide electroreduction, a green technology for artificial carbon cycle, is facing great challenges in designing efficient electrodes. The preliminary research mainly focused on electrodes assembled with powder catalysts and binders, which suffers from high interfacial resistance and insufficient exposure of active sites. Herein, a self-supporting BiIn alloy membrane with nano-thickness was grown in-situ on carbon paper by using the Joule-heating method. The millisecond temperature change (>6000 °C s −1 ) suppresses particles' coarsening and enables the membrane forming with high surface free energy, supplying optimal active sites with special electronic structure to promote CO 2 electroreduction to formic acid. In the H cell, the Faraday efficiency (FE) of formate reaches 100 % at −1.3 V vs the reversible hydrogen electrode. In a solid electrolyte cell, electrolyte-free formic acid was continuously produced for 120 h at −100 mA·cm −2 with FE higher than 90 %. In the alloy phase, the p -band centers of Bi and In were brought closer to their Fermi energy levels strengthen the adsorption of intermediate *OCHO and reduce the energy barrier of HCOOH formation. This work provides a new idea to fabricate binder-free electrodes with three-dimensional conductive skeleton for advanced electrochemical synthesis.
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ACS Nano
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2025
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IF 16
Xuan Zheng,Yi Lu,Jingwen Hu,Zechao Zhuang,Wenchao Zhang,Han Zhu
Electrochemical CO2 reduction (CO2RR) to multicarbon (C2) products provides a compelling pathway for carbon recycling and sustainable energy storage, yet achieving high C2 selectivity remains a major challenge due to kinetic preference for C1 products and the intrinsic difficulty of C–C bond formation. While bimetallic alloys are widely used to tune catalytic performance, their typically random atomic arrangements hinder precise control over active site electronic environments, leading to suboptimal C1/C2 selectivity. Herein, we present a composition-dependent phase engineering strategy to synthesize ordered Au1Cu1 intermetallic alloy, alongside disordered Au3Cu1 and Au1Cu3 alloys, via a polymer nanofiber-mediated approach. The long-range atomic ordering in Au1Cu1 enables an optimized d-band center, critically balancing intermediate binding (e.g., *CO at −1.09 eV) for efficient C–C coupling over C1 formation. This resulted in the Au1Cu1/CNFs catalyst reaching a peak Faradaic efficiency of 55.6% toward C2 products at −0.5 V vs RHE. In situ characterizations and theoretical calculations confirm that its specific electronic and geometric configurations facilitate the lowest energy barrier for *CHO–*CO coupling. This work demonstrates precise atomic-level control in bimetallic alloy ordering, guiding the CO2RR toward valuable multicarbon products.
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PubMed
高影响因子
Frontiers in Energy
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2024
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IF 3.1
Zhang Chen,Zhang Duoyong,Zhang Xinqi,Tian Yongqiang,Wang Liwei
Mesoporous biochar (MC) derived from biomass is synthesized using a dual-salt template method involving ZnCl 2 and KCl, followed by impregnation with polyethyleneimine (PEI) of varying average molecular weights under vacuum conditions to construct a core-membrane structure for enhancing carbon capture performance. The resulting MC exhibits a highly intricate network of micropores and abundant mesopores, along with defects in graphitic structures, effectively facilitating robust PEI loading. Among the PEI-modified samples, PEI-600@MC demonstrates the highest CO 2 sorption capacity, achieving approximately 3.35 mmol/g at 0.1 MPa and 70 °C, with an amine efficiency of 0.32 mmol CO 2 /mmol N. The introduction of amine functional groups in PEI significantly enhances the sorption capacity compared to bare MC. Additionally, PEI with lower average molecular weights exhibits a superior sorption performance at low pressures but shows a reduced thermal stability compared to higher molecular weight counterparts. The area of sorption hysteresis loops gradually decreases with increasing temperature and average molecular weight of PEI. The equilibrium sorption isotherms are accurately modeled by the Langmuir equation, revealing a maximum sorption capacity of approximately 3.53 mmol/g at 70 °C and saturation pressure. This work highlights the potential of dual-salts templated biomass-derived MC, modified with PEI, as an effective, widely available, and cost-efficient material for CO 2 capture.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Yu-Shuai Xu,Hong-Hui Wang,Qi-Yuan Li,Shi-Nan Zhang,Si-Yuan Xia,Dong Xu,Wei-Wei Lei,Jie-Sheng Chen,Xin-Hao Li
The development of two-dimensional heterogeneous catalysts with highly exposed active site areas for heterogeneous catalytic systems is highly promising for achieving the green transformation of small molecules. 2D transition metal carbides (TMCs) show great promise for catalysis and carbon capture but suffer from heavy aggregation and autooxidation. Mass transfer barrier is also a standard problem of lamellar TMCs caused by slight aggregation of layers. Here, we successfully developed a method to prepare “ladder-like” heterojunctions of Mo 2 C layers confined inside nitrogen-rich carbon sheaths (2D-Mo 2 C@NC) via an effective oxygen-diffusion etching strategy, acting as efficient catalysts for CO 2 fixation. The enhanced electron enrichment of the as-integrated 2D-Mo 2 C subunits induced by the Schottky barrier could further keep the exposed Mo 2 C surface from possible autooxidation and aggregation confronted by conventional 2D TMCs. The experimental results and density functional theory (DFT) calculation further demonstrate that electron-rich Mo 2 C could boost the adsorption and activation of CO 2 for universal carbonylation of various diamines, providing a turnover frequency value (TOF) of 10.2 h −1 to produce benzimidazolone, which is 5.2 times of that of the state-of-the-art catalyst in the literature under even critical conditions.
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高影响因子
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