INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Xining Guo,Huiying Li,Leshi Zhang,Rui Hao,Fei Ye,Jianmin Gu,Kaihang Sun,Guozhu Li,Ji−Jun Zou,Zhourong Xiao,Desong Wang
The photothermal catalytic conversion of CO2 into value-added chemicals is of great significance for realizing the goal of carbon neutralization. However, these catalysts have problems such as an insignificant photothermal effect and high recombination of photogenerated carriers. Here, porous TiO2 was prepared by hydrothermal crystallization and topological conversion of metal–organic frameworks (MOFs), and loaded with highly dispersed Pt catalysts to realize an efficient photothermal catalytic reverse water-gas shift (RWGS) reaction. N2-adsorption results showed that the as-prepared Pt/TiO2 catalysts had an abundant mesoporous structure, thus contributing to the rapid diffusion of reactants and light transport. X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) results showed that Pt was uniformly dispersed on the catalyst surface with an average particle size of 2.06 nm. H2-TPR profiles showed that the Pt/TiO2 catalyst had strong metal–support interactions, CO2-TPD showed its strong CO2 adsorption capacity, and CO-TPD showed its weak CO adsorption strength. In situ X-ray photoelectron spectroscopy (XPS) showed that the electron cloud density on the Pt surface further increased under light illumination, which contributed to the activation and dissociation of H2. In addition, the Pt/TiO2 catalyst had a narrow band gap width and sufficiently low reduction potential, and its excellent photothermal and photovoltaic properties ensured efficient performance in the photothermal RWGS reaction. The Pt/TiO2 catalysts showed a high CO2 conversion of 29.8%, a product CO selectivity higher than 99.6%, and a stability of more than 3000 min at 350 °C, with a light intensity of 1.2 W cm–2 and a GHSV of 36,000 mL gcat–1 h–1.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Xu Feiyan,Zhao Feifan,Deng Xianyu,Zhang Jinfeng,Zhang Jianjun,Ai Chenbin,Yu Jiaguo,García Hermenegildo
The rapid increase in atmospheric CO 2 levels due to industrialization underscores the urgent need for innovative carbon valorization strategies. Photocatalytic CO 2 reduction presents a sustainable solution; however, conventional systems suffer from inefficient charge separation and limited product applicability. Herein, a green and scalable tandem strategy is developed by integrating S-scheme photocatalysis with palladium-catalyzed carbonylation. A rationally designed CeO 2 /Bi 2 S 3 heterojunction leverages its hierarchical structure, broad visible-light absorption, oxygen-vacancy-mediated charge dynamics, and the S-scheme charge transfer mechanism to achieve highly efficient photocatalytic CO 2 -to-CO conversion (14.05 mmol g −1 , 98% selectivity). The generated CO is directly utilized in a subsequent carbonylation reaction under mild conditions, yielding high-value amides with near-quantitative CO utilization. This integrated approach eliminates the risks of CO handling and enhances economic viability, providing a direct and effective route for converting CO 2 into fine chemicals. By bridging photocatalysis with industrial catalysis, this work advances sustainable carbon recycling technologies and opens avenues for the development of efficient CO 2 conversion systems.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-14
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IF 15.7
Zhang Fanxing,Cao Ning,Wang Chentao,Wang Shengxiang,He Yi,Shi Yao,Yan Mi,Bao Ying,Li Zhenglong,Xie Pengfei
Electrochemical CO 2 -to-ethanol conversion is challenged by sluggish C-C coupling kinetics and wide products distribution. Although Cu + has been demonstrated to enhance multi-carbon (C 2+ ) formation, the stabilization of Cu + under reduction conditions is difficult. Here, we report a hydrogen-ethanol pretreatment strategy to obtain Cu nanoparticles covered by highly dispersed and disordered ZnO 1- x clusters. Ethanol-induced ZnO 1- x redispersion gives rise to abundant Cu + on the subsurface. The optimal catalyst delivers a 73.0% ethanol Faradaic efficiency (FE) and 86.0% total C 2+ FE at −0.9 V, with a 2.3 mmol cm −2 h −1 ethanol formation rate and single-pass ethanol yield of 18.0%. The catalyst also exhibits stability beyond 500 h, attributed to the stabilization of Cu + by the ZnO 1- x shield that requires a high energy barrier for lattice oxygen removal. In situ X-ray spectroscopy and calculations reveal a volcano relationship between Cu + ratio in Cu species and ethanol FE. Optimal Cu + density not only facilitates *OC-COH coupling but also optimizes the adsorption energy of *CH 2 CH 2 O on catalyst for ethanol electrosynthesis.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Tao Pu,Yanping Li,Xiujuan Yang,Ran Ao,Quxiu Dai,Jie Yang,Zhiying Guo,Liping Ma,Zhanghong Wang
Silicoaluminophosphate-20 (SAPO-20) molecular sieve was synthesized from solid waste coal gangue (CG) and aluminum ash (Al-ash), and its adsorption capacity for CO 2 was evaluated. The content of Si and Al in raw materials was increased by hydrochloric acid pretreatment, and the synthesis conditions (NaOH/CG ratio, calcination temperature, hydrothermal reaction temperature and time, liquid–solid ratio) were optimized by single factor analysis. The synthesized products were characterized by XRD, SEM, BET, FTIR and TEM. The results showed that the SAPO-20 crystal form prepared under the optimal conditions had high purity, BET surface area of 175 m 2 /g, and pore structure with multistage pore distribution, which was conducive to gas diffusion and adsorption. Thermogravimetric analysis revealed that under the conditions of 25 °C and 1 bar, compared with the CO 2 adsorption capacity of 5.63 mg/g for CG, the CO 2 adsorption capacity of SAPO-20 was 27.92 mg/g. The adsorption process was in line with the Langmuir monolayer model and had exothermic characteristics (ΔH = –152 kJ/mol). The adsorption kinetics was fitted by Pseudo-First-Order Kinetic Model (R 2 = 0.740–0.995), and the adsorption rate increased with the increase of temperature. In addition, compared with the traditional synthesis method, the synthesis cost of this study was reduced by more than 70 %, and the carbon emission was reduced by about 75 %, realizing economic and environmental viability.
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Catalysis Science & Technology
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2025
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IF 4.2
Congyu Qin,Shuchen Xing,Guiming Ba,Huilin Hu,Jinhua Ye,Defa Wang
Photothermocatalytic carbon dioxide (CO2) reduction into value-added chemicals is one of the promising methods for solar-to-chemical energy conversion. However, it remains a challenge in the improvement of catalytic activity and product selectivity in view of practical applications. Herein, we report a facile “two-step” approach – nitrogen treatment of Ti3C2 MXene (TC) and loading of Co nanoparticles – to synthesize a Co-nanoparticle/layered TiO2-TiN (Co/TiO2-TiN) composite as an efficient photothermocatalyst for selective reduction of CO2 to methane (CH4). In contrast to the Co/Ti3C2 catalyst that shows a high CO selectivity, the optimal 35Co/TiO2-TiN catalyst exhibits a CH4 evolution rate of 45.5 mmol gcat−1 h−1 with 99.3 % selectivity under a 300 W Xe lamp irradiation. The synergistic effect of increased light absorption capacity, reactive sites, CO2 adsorption/activation ability, and desorption energy barrier of CO* intermediate by the loaded Co nanoparticles and the formation of Ti−N−O bonds accounts for the significantly enhanced photothermocatalytic performance of 35Co/TiO2-TiN for selective CO2 reduction into CH4. Our work demonstrates that metal nanoparticle loading and formation of Ti−N−O bonds can be integrated into the strategy in developing a photothermocatalyst for efficient CO2 reduction with controlled product selectivity.
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Science Advances
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2025
·Vol. 11
·期 32
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IF 12.5
Congcong Yin,Muning Chen,Ziyin Zhang,Kai Liu,Jinglin Gao,Xin Zhao,Yuping Wu,Yong Wang
Creation of membrane channels capable of recognizing diverse molecules is desirable for advancing molecular transport and separation, but it remains difficult to precisely control their conformation and achieve dynamic adaption to specific molecules. Here, we demonstrate fine-tuning the pore environment within 3D covalent organic framework (COF) that can precisely control its pore size and polarity to recognize CO 2 . The pores are integrated with azobenzene units with photo-adaptable trans-to-cis isomerization, enabling dynamic pore size regulation at angstrom scale. Moreover, the isomerization induces drastic changes in intrapore polarity, which exert profound effects on the intermolecular affinity through the dipole-quadrupole interaction. Featuring these dynamic natures, the 3D COF membrane cooperating the size exclusion effect with a molecular recognition ability toward CO 2 . As a result, light-gating separation experiments show the superior CO 2 capture performance with a N 2 /CO 2 selectivity of 27.6. Theoretical calculations reveal that cis-state azobenzene can reduce the electron transfer barrier from azobenzene to CO 2 , thereby providing a molecular recognition pathway.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2025
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IF 4.7
Rou Wen,Qingqing Ye,Qi Wang,Xu Li,Dongfang Guo,Lianbo Liu,Shiwang Gao,Liqiang Luo,Achao Chen,Tong Wu,Meiling Dou
The development of high-efficiency CO 2 separation membranes represents a critical pathway toward achieving the goal of carbon neutrality. In this work, we present a size-controlled strategy to fabricate a high-performance mixed matrix membrane (MMM) using poly (vinylamine) (PVAm) matrices incorporated with zeolitic imidazolate framework (ZIF-8) filler (size range: 98-1200 nm). Systematic investigation reveals that ZIF-8 particle size critically governs interfacial compatibility with the PVAm matrix, directly impacting CO 2 separation efficiency. Both significantly larger or smaller particles than 130 nm tend to induce non-selective interfacial voids at the polymer-filler interface. Optimal performance is achieved with 130 nm ZIF-8 fillers, which exhibits superior dispersion stability in PVAm solutions, as evidenced by the highest zeta potential values. The resultant MMM exhibits high separation performance under 0.1 MPa feed pressure, achieving a CO 2 permeability of 455.06 GPU and CO 2 /N 2 selectivity of 42.36, higher than those of the pure PVAm-based membrane without ZIF-8 filler. This work provides valuable guidance for the design of high-performance CO 2 separation membranes, advancing the development of sustainable carbon management technologies.
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CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Ruijie Ma,Huimin Gao,Jinpeng Zhang,Jieying Jing,Wen-Ying Li
Photocatalytic reduction of CO 2 to formic acid (HCOOH) offers a sustainable pathway for carbon utilization, yet its efficiency is fundamentally limited by poor CO 2 adsorption and rapid electron-hole recombination in conventional photocatalysts. To address this challenge, a series of Pd-loaded hydrogenated TiO 2 catalysts (x wt%Pd/H-TiO 2 ) were developed through a synergistic hydrogen reduction-impregnation strategy, aiming to regulate the electron density of Pd active sites and enhance interfacial charge separation. Systematic characterization revealed that increasing Pd loading (0.6–1.4 wt%) effectively trapped photogenerated electrons, suppressing recombination losses and elevating electron density at Pd sites. Combined with optimized CO 2 adsorption capacity (0.178 mmol·g −1 ) and accelerated charge transfer, the 1.0 wt%Pd/H-TiO 2 catalyst achieved a HCOOH production rate of 14.14 mmol·g cat −1 ·h −1 under mild conditions (30 °C, 2.0 MPa, 4.57 mW·cm −2 ), outperforming most reported TiO 2 -based systems. Mechanistic studies further demonstrated a strong correlation between Pd-induced electronic effects and multi-electron CO 2 activation kinetics. This work provides a scalable catalyst design paradigm for balancing charge dynamics and surface reactivity in photocatalytic CO 2 valorization.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Man Zhao,Wei Wen,Chunmei Liu,Qinyun Yan,Shuai He,He Xiao,Li Zhang,Junming Zhang,Xiaofeng Gao,Jianfeng Jia
The electrochemical CO 2 reduction reaction (CO 2 RR) to multi‑carbon products offers a promising route for sustainable fuel production, yet achieving high selectivity remains challenging due to the complex interplay between catalyst structure and reaction pathways. Here, we report a rational design of Cu-Cu 2 O/graphene (Cu/G) composites with tunable Cu + /Cu 0 ratios via electrolyte-mediated electrochemical synthesis. By varying tetraalkylammonium/phosphonium electrolytes (TBABF 4 , TBAPF 6 , TBACF 3 SO 3 , TBPBF 4 ), we precisely control Cu oxidation states, as validated by the results of X-ray absorption fine structure (XAFS), X-ray diffraction (XRD), and high-resolution transmission electron microscope (HRTEM). In-situ Fourier transform infrared (In-situ FTIR) spectra and in-situ Raman spectra indicate Cu + -rich surfaces (Cu/G-TBABF 4 ) favor the production of formate via O-bound intermediates, while Cu 0 -dominated interfaces (Cu/G-TBAPF 6 ) promote the formation of CO through C-bound pathways. Mixed Cu + /Cu 0 systems (Cu/G-TBACF 3 SO 3 , Cu/G-TBPBF 4 ) enable C C coupling, with ethylene (FE = 28 %) and ethanol (FE = 30.2 %) selectivity governed by the Cu + /Cu 0 balance. Ultraviolet photoelectron spectroscopy (UPS) results reveal that lower work functions enhance *CO coverage and stabilize C 2+ intermediates, elucidating the electronic structure-activity relationship. This work demonstrates electrolyte-mediated oxidation state engineering as a versatile strategy to steer CO 2 RR pathways, offering a generalizable approach for designing multi-valent electrocatalysts with tailored selectivity.
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Nanoscale
·
2025
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IF 5.1
Yubin Zheng,Zhe Lu,Zhisheng Shi,Lu Wang,Shuyuan Yang,Runzhi Cao,Gao Wa,Xin Zhou,Yong Yang,Chong Sheng,Yong Zhou,Zhigang Zou
A highly dispersed NiCo alloy catalyst derived from NiCo bimetallic–organic framework nanosheets was synthesized for efficient photothermal catalysis for CO2 hydrogenation to methane. The NiCo bimetal catalyst achieves a CH4 production rate of 55.60 mmol g−1 h−1 with only a 18.82% decline in performance after 86 hours under atmospheric pressure at selected 290 °C and continuous flow reaction. In situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) reveals the synergistic and complementary roles of light and heat in photothermal catalysis. The thermochemical process drives the reverse water–gas shift reaction to form a *CO intermediate, a key intermediate for the formation of CH4, and light irradiation-generating strong near field from the surface plasma resonance of NiCo bimetals promotes the subsequent *CO hydrogenation step to form *CHO, the rate-determining step for the hydrogenation of CO2 into CH4. Meanwhile, density functional theory (DFT) calculations suggest that the NiCo bimetallic catalyst can also lower the energy barrier of *CO hydrogenation, facilitating the formation of *CHO.
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ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Xinmei Wang,Junqiang Han,Jianing Ni,Jianan Li,Chang Gao,Changlei Qin
Spent lithium-ion batteries (LIBs) are expected to be discarded in huge amounts due to their limited service life, causing severe environmental problems if not properly handled. It is a promising route to obtain cheap CO2 separation materials of Li-based CO2 sorbents and Ni/Mn/Co-based oxygen carriers from spent ternary LIBs, realizing a win-win outcome in terms of waste recycling and CO2 reduction. However, the migration of key impurities during the recycling of spent LIBs and the approach to synthesizing CO2 separation materials may affect their physical and chemical characteristics. Herein, the work aims to develop CO2 separation materials from spent ternary LIBs, elaborating the migration and influence of impurities, and optimizing the performance of CO2 separation materials. Results show that Ni, Co, and Mn in spent LIB cathode enter oxygen carriers with a minor amount of Li, Al, etc., while Li mainly enters Li4SiO4 sorbents with some Na and Si. After optimization, the obtained oxygen carrier of CO–OC-0.3Al possesses a stable oxygen transport capacity of 16.3% during 30 cycles of reduction and oxidation, and the sorbent of CO-Li4SiO4-0.1Na could attain an excellent CO2 capacity of 0.26 g/g within 100 cycles of adsorption and desorption. We believe that the work could lay a foundation for the efficient construction of CO2 separation materials from spent LIBs, which is of great significance for environmental protection and low-carbon energy development.
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ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Kai Zhu,Zihan Lin,Xinyi Bai,Fangfang Chang,Qing Zhang,Xiaolei Wang,Zhengyu Bai
Electrocatalytic reduction reaction of CO2 (CO2RR) into value-added multicarbon (C2+) products represents a sustainable strategy for mitigating greenhouse gas emissions and enhancing the production of high-value chemicals. Cu-based catalysts are optimal for the CO2RR, facilitating the generation of C2+ products such as ethanol, which have significant industrial applications. However, converting CO2 to C2+ products remains a great challenge, necessitating the simultaneous achievement of high current density, Faradaic efficiency (FE), and operational stability for industrial-scale implementation. Herein, we prepared Cu/Cu2O catalysts with diverse morphologies and the ratio of the Cu+/Cu interface, which was rectified by regulating the interactions between the active interface and the intermediate (*CO). The electrochemical analysis demonstrated that reconstructed Cu/Cu2O nanodendrites with dominant grain boundaries exhibited remarkable performance in generating C2+ products, achieving a Faradaic efficiency (FE) of 71.8%, including 49.7% FE of ethanol and a substantial partial current density of 390.0 mA cm–2 within the flow cell. In situ spectroscopy characterization and theoretical calculations revealed that the increased ethanol selectivity originated from the rectification of the Cu/Cu2O interface by the *CO intermediate, which accelerated H2O dissociation, reduced the free energy for *CO hydrogenation to *COH, and facilitated asymmetric *CO-*COH coupling to preferentially reduce CO2 to ethanol. This study provides profound insights into the C–C coupling pathways and sheds light on the rational design of ethanol-oriented electrocatalysts, contributing to sustainable chemical synthesis and energy utilization.
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