JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Shihao Xiong,Tao Peng,Liangliang Huang,Rui wang,Beibei He,Jun Jin,Huanwen Wang,Yansheng Gong
Semiconductor photocatalytic nitrogen reduction reaction (PNRR) stands as a promising clean technique for ammonia synthesis, yet it confronts numerous challenges. In this study, Ag nanoparticle-modified Cu-doped Bi 2 WO 6 (ACB) porous composite materials with varying mass percentages were successfully synthesized using a solvothermal reduction approach. The incorporation of transition metal Cu effectively modulates the energy band position of Bi 2 WO 6 . Furthermore, the introduction of Ag nanoparticles significantly suppresses the recombination of photogenerated carriers. Without adding sacrificial agent, the photocatalytic nitrogen fixation yield of ACB reaches an impressive 184.93 μmol·g −1 ·h −1 , which is 5.44 times higher than that of pristine Bi 2 WO 6 . A comprehensive analysis of the experimental results reveals that the combined effect of Cu doping and Ag nanoparticle loading endows ACB with an increased exposure of active sites, thereby significantly enhancing its photocatalytic nitrogen fixation performance. This research offers a promising approach for the design of metal nanoparticle-supported catalysts for PNRR, holding significant implications for the advancement of other material systems.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shengjun Du,Minglong Guo,Guangxing Yang,Qiao Zhang,Zhiting Liu,Feng Peng
The highly-efficient separation of CH 4 /N 2 mixture on carbon materials is significantly hindered by the inherent trade-off that exists between CH 4 adsorption capacity and CH 4 /N 2 separation selectivity. Herein, we have constructed a type of novel carbon materials (PGC- x ) with well-controlled ultramicropores ranging from 0.48 to 0.57 nm for CH 4 /N 2 separation. The Zn-based salt template was in-situ confined into the polymer framework during the co-assembly of phloroglucinol and glyoxylic acid. The subsequent evaporation of Zn at high temperature gives rise to the adjustable ultramicropore structure, effectively devoid of mesopores and macropores. Benefiting from the optimal pore size of 0.50 nm, PGC-1 demonstrated high CH 4 uptake of up to 1.50 mmol/g. Meanwhile, the CH 4 /N 2 (15/85 and 85/15, v/v) separation selectivity of PGC-1 at 298 K and 1.0 bar reached 5.8 and 6.0, respectively. Dynamic breakthrough experiments proved that PGC-1 could be used as efficient adsorbent for capturing low or high concentration of CH 4 from N 2 . This work offers a promising design principle for optimizing porous structure of carbon materials, with the aim of minimizing the selectivity-capacity trade-off that often arises in the separation of diverse gas pairs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Mao Ye,Hexiang Huang,Lei Tian,Xiujing Zhang,Ziyao Wang,Chenxu Zhang,Zhihua Qiao
Separation of CH 4 and N 2 from natural gas is essential to increase energy efficiency and reduce environmental impact. In this work, we prepared novel mixed matrix membranes (MMMs) for CH 4 /N 2 separation using ion-exchange-modified molecular sieves as fillers and metal–organic framework (MOF) glass as substrates. The modification of molecular sieves enhanced the gas separation capability of the MMMs. And the MOF glass as a matrix has good compatibility with the filler. The membrane achieved a CH 4 permeance of up to 271.4 GPU and a CH 4 /N 2 selectivity of 7.35. The membrane was able to maintain stable separation performance under certain pressures and over a long testing period. The design of this study provides an innovative approach to advancing natural gas applications.
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INORGANIC CHEMISTRY
·
2026
·Vol. 65
·期 29
·16879-16886
·
IF 4.6
Wu Jing,Wang Ruonan,Lin Haifeng,Xing Jun,Wang Lei,Xu Jixiang
In this work, a novel ternary heterojunction consisting
of Zn vacancy-rich
zinc oxide (Zn 1– x O), a zeolitic
imidazolate framework-8 (ZIF-8), and cobalt phthalocyanine (CoPc)
was fabricated for photocatalytic N 2 fixation. The Zn 1– x O/ZIF-8 composite with bridged O–Zn–N
bonding was synthesized via in situ growth of ZIF-8 on Zn 1– x O, and it possessed a large surface area favorable
for N 2 adsorption. The incorporation of CoPc with dispersed
Co–N 4 (II) sites enhanced light harvesting and N 2 activation. Zn vacancies and coupled type II/Z-scheme charge
transfer pathways in the heterojunction accelerated the separation
of photogenerated charge carriers. As a result, the optimized catalyst
exhibited superior and stable photocatalytic N 2 reduction
performance via an alternating pathway in water, with an NH 4 + production rate of 65.2 μmol g –1 h –1 , which is 17.0 times higher than that of ZnO.
This study develops a novel ZnO-based heterojunction that simultaneously
optimizes multiple key factors for efficient photocatalytic N 2 fixation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Jia Wang,Yizhen Situ,Wenyu Zheng,Weidong Zhang,Qingyuan Yang
Polymer transport resistance was tuned by controlling the solvent evaporation rate. • Reduced polymer transport resistance promoted a more effective contribution of ZIF-8 transport pathways to CO 2 /N 2 separation. • The 7.8 wt% in situ-grown MMM achieved a CO 2 permeability of 510 Barrer and a CO 2 /N 2 selectivity of 33.0. Beyond filler modification, regulating the polymer structure is also crucial for optimizing gas transport in mixed-matrix membranes (MMMs), yet this aspect remains insufficiently explored. Herein, the solvent evaporation rate was controlled to regulate the transport resistance of Pebax 2533 and elucidate its influence on the transport contribution of ZIF-8 in ZIF-8/Pebax MMMs for CO 2 /N 2 separation. For Pebax 2533 membranes, increasing the evaporation rate reduced both crystallinity and relative fractional free volume, resulting in a non-monotonic variation in CO 2 permeability and a decrease in CO 2 /N 2 selectivity. At a moderate evaporation rate of 2.5 × 10 −5 kg·m −2 ·s −1 , the balance between reduced crystallinity and preserved free volume resulted in lower polymer transport resistance, enabling the contribution of ZIF-8 to be more effectively translated into membrane separation performance. As a result, the in situ-grown MMM containing 7.8 wt% ZIF-8 achieved a CO 2 permeability of 510.0 Barrer and a CO 2 /N 2 selectivity of 33.0, with its CO 2 permeability exceeding that of most reported Pebax-based MMMs. This work demonstrates that controlling solvent evaporation is an effective strategy to regulate polymer transport resistance and enhance the contribution of ZIF-8 in MMMs. Download: Download high-res image (207KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jinyu Liu,Nan Zheng,Xiaoli Dong,Yubo Zhang,Xinyue Liu
Y-doped SrTiO 3 nanosheets were developed for piezophotocatalytic N 2 fixation. • 3%Y-SrTiO 3 achieves a robust ammonia yield of 642.66 μmol·g −1 ·h −1 under combined piezoelectric and visible-light excitation. • Piezoelectric field and oxygen vacancies synergistically boost charge separation and N 2 activation. Piezoelectric-assisted photocatalysis offers a sustainable route for N 2 fixation, but is often hampered by weak piezoelectric polarization and insufficient N 2 chemisorption/activation sites. Herein, we introduced aliovalent Y-doping into SrTiO 3 to induce lattice distortion for enhanced piezoelectric response and generated abundant oxygen vacancies for N 2 chemisorption. The optimized 3%Y-STO achieves a remarkable NH 3 yield of 642.66 μmol·g −1 ·h −1 under dual piezocatalytic and visible-light (PE/Vis) excitation. PFM measurements confirm the significantly improved piezoelectricity, and the resulting polarization field drives efficient carrier separation. DFT calculations reveal that Y-induced oxygen vacancies serve as active sites for N 2 adsorption, while the piezoelectric polarization facilitates the activation of adsorbed N 2 . This synergy between piezo-driven charge separation and defect-mediated N 2 activation enables efficient N 2 reduction. This work validates aliovalent doping as an effective dual-function strategy for sustainable piezophotocatalytic N 2 fixation. Download: Download high-res image (236KB) Download: Download full-size image
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JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Peipei Zhou,Caiyan Zhang,Liting Yu,Yongyan Deng,Lu Qiao,Meng Wang,Lili Fan,Daofeng Sun,Alex C.K. Yip,Zixi Kang,Xiaoqin Zou
SSZ-13 zeolite membranes are promising for N 2 /CH 4 gas separation owing to their unique pore architecture and superior stability. However, for the conventional secondary growth (CSG) of SSZ-13 membranes, the synthetic solution, particularly the organic template, is inefficiently utilized, causing unnecessarily high chemical consumption. To address this issue, this study introduces counter-diffusion crystallization (CDC) strategy that separates the organic template and silica source within and outside porous tube substrates to synthesize SSZ-13 membranes at the interface; this can reduce template usage by 92.5% for the same area of SSZ-13 membranes compared with the CSG method. Moreover, with the CDC strategy, the organic template can be recycled for membrane fabrication, further reducing raw material costs. The optimized SSZ-13 membranes show N 2 permeance of 2.5 × 10 −8 mol m −2 s −1 Pa −1 and N 2 /CH 4 selectivity of 15.7 at 298 K and 2 bar. Meanwhile, SSZ-13 membranes can maintain stable performance over one month of operation and be able to withstand high-temperature (423 K) and high-pressure (10 bar) tests.
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Science China-Chemistry
·
2026
·
IF 9.8
Liu Zhaozhuang,Wang Mingxi,Wang Li,Liu Jiaqi,Li Jinping,Yang Jiangfeng
The efficient separation and enrichment of methane (CH 4 ) from low-concentration coalbed methane (CBM) are of great significance for enhancing CBM utilization efficiency and promoting the development of low-carbon clean energy. To address this practical need, this study synthesized a tailored chlorinated metal-organic framework (MOF), PCP-IPA-Cl, and systematically evaluated its CH 4 /N 2 separation performance through a combination of static adsorption measurements, density functional theory (DFT) calculations, dynamic breakthrough experiments, and multiple adsorption-desorption cycling tests. Endowed with its optimized pore structure and chlorinated channel environment, PCP-IPA-Cl exhibits excellent CH 4 /N 2 separation performance and regeneration stability: at 298 K and 1 bar, it achieves a high CH 4 adsorption capacity of 21.27 cm 3 /g with a low N 2 uptake of only 5.29 cm 3 /g, and compared with its unchlorinated analog PCP-IPA, the CH 4 /N 2 selectivity is markedly improved from 5.4 to 9.0. DFT calculations reveal that the introduction of–Cl groups creates additional preferential adsorption sites for CH 4 molecules, strengthening host-guest interactions and thus enhancing separation efficiency. Furthermore, breakthrough experiments confirm its excellent dynamic separation ability, and cyclic tests demonstrate that PCP-IPA-Cl can be fully regenerated via helium purging within just 5 min. These findings collectively demonstrate that PCP-IPA-Cl is a promising and regenerable adsorbent for the efficient enrichment and utilization of low-concentration CBM.
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Journal of Energy Chemistry
·
2026
·
IF 15.6
Shengxi Zhao,Linyan He,Jinquan Li,Da Song,Juan Fu,Si Lu,Zhen Huang,Fang He
Ammonia is a crucial chemical and carbon-free energy carrier, but its industrial synthesis via the Haber–Bosch process requires harsh conditions and fossil-derived hydrogen. Alternative strategies are needed to achieve sustainable ammonia production under moderate conditions. H 2 O-based chemical looping ammonia synthesis (H 2 O-CLAS) enables hydrogen-free operation and decouples N 2 and H 2 O activation from scaling constraints, but remains hindered by high energy demand, inferior catalyst stability, and intrinsically challenging activation of N 2 and H 2 O. Here we demonstrate Co-doped LaMnO 3 as a durable and efficient H 2 O-CLAS catalyst, where nitrogen fixation occurs at 1000 °C and ammonia release proceeds at 600 °C under atmospheric pressure with a production rate of 866.01 µmol g −1 h −1 , outperforming state-of-the-art H 2 O-CLAS catalysts. Co doping modulates the d-band electronic structure of LaMnO 3 via spin-state engineering and enhances lattice oxygen mobility, thereby promoting N 2 and H 2 O activation, nitride formation, and hydrogen-bond interactions for ammonia formation. This work outlines a pathway toward sustainable ammonia synthesis with markedly reduced energy consumption and carbon emissions. Scheme. Illustration of spin-state modulation in Co-doped LaMnO 3 for chemical-looping ammonia synthesis. Download: Download high-res image (216KB) Download: Download full-size image
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Catalysts
·
2026
·Vol. 16
·期 6
·512
·
IF 4.5
Xinlu Xiong,Donglin Song,Qiang Ren,Xu Xiang,Jiongliang Yuan
The electrocatalytic reduction in N2and CO2into urea under ambient conditions provides a promising strategy for sustainable nitrogen fixation and carbon utilization. However, the low activity and poor selectivity toward urea limit its practical application. Herein, a dual-ligand Cu-based metal–organic framework (Cu-BTC/NH2BDC) was constructed via ligand engineering strategy. The introduction of 2-NH2BDC modulated the electronic structure of Cu sites, generating electron-enriched Cu centers that facilitate CO2activation, while the hydrogen bonding interaction between the amino and carboxyl groups promotes the activation of N2. As a result, the optimized Cu-BTC/NH2BDC catalyst achieved a urea yield of 6.59 mmol g−1h−1with a Faradaic efficiency of 22.85% at −0.2 V versus reversible hydrogen electrode (vs. RHE), outperforming single-ligand counterparts. In situ Raman spectroscopy measurement revealed enhanced the formation of *CO, *NN, and C-N intermediates, indicating improved C-N coupling efficiency. This work provides a feasible strategy for regulating active sites in MOF-based catalysts toward efficient urea electrosynthesis.
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INORGANIC CHEMISTRY
·
2026
·Vol. 65
·期 35
·20723-20730
·
IF 4.6
Cong Shenzhen,Sun Si,Wang Ming,Zhang Yijing,Shen Qin,Zhang Yatao,Pang Huan
Membrane-based separation technology holds great promise
for CO 2 capture, yet conventional membranes are often constrained
by the permeability-selectivity trade-off. In this study, we developed
a zirconium-cluster (Zr 6 )-incorporated ZIF-8 membrane via
an electrochemical synthesis strategy to address this limitation.
The resulting Zr 6 @ZIF-8 composite membrane exhibits high
crystallinity, a dense microstructure, and homogeneous dispersion
of Zr 6 clusters within the ZIF-8 framework. The optimized
Zr 6 @ZIF-8–2 membrane demonstrates outstanding CO 2 separation performance with a CO 2 permeance of
up to 300.0 gas permeation unit and CO 2 /N 2 and
CO 2 /CH 4 selectivities of 27.0 and 14.8, respectively.
The Zr 6 clusters enable effective structural regulation
of ZIF-8 membranes, resulting in enhanced CO 2 separation
performance and leading to improved diffusion selectivity. Furthermore,
the membrane shows a stable separation performance under varying feed
pressures and temperatures, along with excellent long-term operational
stability. This work provides an effective electrochemical approach
for fabricating high-performance MOF-based membranes, offering a promising
candidate for industrial CO 2 capture and natural-gas purification.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Beining Qi,Shangzhen Zhang,Qingze Shi,Zexuan Gong,Qian Yue,Zhenqi Duan,Tianyi Zhang,Yinglong Wang,Limei Zhong,Fengbin Zheng
A rapid and easily scalable solvothermal method is developed to synthesize UiO-66 with different functional groups. • UiO-66-NH 2 exhibits excellent CO 2 /N 2 separation performance. • UiO-66-NH 2 significantly enhances the adsorption interaction with CO 2 . • This solvothermal method exhibits good scalability and performance reproducibility. UiO-66 is one of the most promising metal-organic framework (MOF) materials for CO 2 adsorption due to its high specific surface area, high stability, and ease of functionalization. However, its synthesis methods often suffer from problems such as long reaction times, uneven mass and heat transfer, and limitations in equipment size. Here, we develop a rapid and easily scalable solvothermal method to prepare UiO-66 with different functional groups, denoted as UiO-66-x (x = H, NH 2 , NO 2 , F, CH 3 ), for the selective separation of CO 2 and N 2 . Adsorption experiments show that UiO-66-NH 2 exhibits excellent adsorption performance for CO 2 , reaching an adsorption capacity of 76.71 cm 3 /g at 273 K and 0.1 MPa, which is superior to some reported solid adsorbents. Dynamic breakthrough experiments show that UiO-66-NH 2 has excellent separation performance for CO 2 and N 2 under practical conditions. More importantly, UiO-66-NH 2 exhibits good reusability after 10 consecutive adsorption-desorption cycles. Theoretical calculations indicate that the introduction of amino groups enhances the adsorption interaction of UiO-66-NH 2 with CO 2 , thereby improving its selective adsorption capacity. Furthermore, the UiO-66-NH 2 prepared in gram-scale experiments exhibits high consistency with the milligram-scale samples in terms of crystal structure and CO 2 adsorption performance, indicating that this method has good scalability and performance reproducibility. Download: Download high-res image (247KB) Download: Download full-size image
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