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ACS Sustainable Chemistry & Engineering · 2025 · IF 7.3

N-Doped Carbon-Encapsulated Cu@SS-Arg Catalyst for H2 Production from Aqueous-Phase Reforming of Ethanol: Toward Carbon-Neutral Energy Cycles

Minglei Lu,Bo Zhang,Shuting Jiang,Xuezhao Yu,Yingying Zhong,Junwei Liao

The development of high-performance catalysts for aqueous-phase reforming of ethanol (APRE) is essential for advancing sustainable hydrogen production and achieving carbon neutrality. Herein, we report a N-doped carbon-encapsulated Cu nanoparticle catalyst (Cu@SS-Arg), which enhances hydrogen selectivity and suppresses carbon-containing gas byproducts. The Cu@SS-Arg catalyst, which has been optimized, achieves a H2 production rate of 31.2 μmol/gcat/s with a H2 selectivity of 99.99% at 210 °C, while concomitantly reducing CO emissions in comparison to commercial precious metal catalysts. In situ DRIFTS and TPSR-MS analyses demonstrate that the Cu+/Cu0 active sites not only promote ethanol/water activation but also facilitate the C–H/O–H bond cleavage, thus favoring the ethanol dehydrogenation (via *CH3CH2O, *CH3CHO, and *CH3COOH intermediates), water dissociation (*H2O → *OH + *H) and carbon monoxide conversion (*CO + *OH → *CO2 + *H) pathways over C–C bond cleavage. This work presents a dual strategy for designing nonprecious metal catalysts that synergistically integrates structural stabilization with N-doping regulation. Together, these approaches enable sustainable and low-carbon production of hydrogen from renewable ethanol.

CAS / MDL: 64-17-5
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Synergy of sulfur vacancy and piezoelectric effect to tune charge migration in Sv-ZnIn2S4/UiO-66-NH2 for efficient photocatalytic H2 evolution

Ming Fang,Zhenfei Yang,Yang Guo,Shuqin Yuan,Xinnian Xia,Shuaijun Pan

High-performance photocatalytic H 2 evolution materials require strong light absorption capability, excellent photogenerated charge separation ability and efficient charge carrier migration capability. In this study, we designed a piezoelectric photocatalytic heterojunction composed of UiO-66-NH 2 and ZnIn 2 S 4 nanosheets with sulfur vacancies. The Sv-UZ-45 heterojunction achieved piezoelectric photocatalytic H 2 evolution performance of 3886.4 μmol·g -1 ·h -1 , with a 4.6 times enhancement due to the synergistic effect of piezoelectric effect and defect engineering. The introduction of sulfur vacancies enables the heterojunction to obtain stronger light absorption, while the higher CB position of rich-sulfur vacancies ZnIn 2 S 4 is more favorable for the photocatalytic reduction reaction. In addition, the heterojunction with rich-sulfur vacancies exhibits a stronger piezoelectric effect than without vacancies, thus providing a powerful driving force for the separation of photogenerated charge carriers. Finally, ESR was used to explain the potential photocatalytic mechanism and showed that Sv-UZ-45 adheres to the Z-scheme carrier migration pathway. This work elucidates the synergistic interaction between piezoelectric effect and defect engineering, providing new insights for the further development of high-performance piezoelectric photocatalysts.

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Nano Energy · 2025 · IF 17.1

S-Pt coordination bond enhanced local surface plasmon resonance boosts photocatalytic H2 production coupled with high value-added products from plastic waste

Ying Wang,Ruolan Zhao,Yachao Xu,Bojing Sun,Zhong Zhou,Peng Yu,Yue Qu,Youxing Liu

Solar driven the conversion of plastic waste, one of emerging environmental pollution sources, into clear energy and high value-added products, is of great significance for human health and sustainable economic development globally, however, still suffer from low reaction kinetics and unsatisfactory selectivity. Herein, we proposed a new strategy of zinc indium sulfide (ZIS) nanosheets anchoring Pt cluster (ZIS-Pt-Clu) for enhancing local surface plasmon resonance (LSPR), by accurately synthesizing S-Pt coordination bond for constructing electron transport channel, for the purpose of promoting the reaction kinetics and selectivity of plastic waste into hydrogen and high value-added products. Experiment shows that the as-made ZIS-Pt-Clu photocatalyst exhibits a high hydrogen production rate of 11.7 mmol h −1 g −1 , together with 97.5 % of selectivity of polylactic acid (PLA) to pyruvic acid (PA), which is the best compare with ZIS/Pt-Clu without hot electron transport channel and reported active materials. In addition, the S-Pt coordination bond also triggers strong interface crystal field between Pt cluster and ZIS to promote the separation and transport of photogenerated carriers, which accelerates the photocatalytic conversion of PLA into H 2 and PA. Overall, this work reportes a new strategy of LSPR enhanced photocatalytic performance, opening the door for the fundamental research of designing high performance photocatalyst for the degradation of plastic waste to the production of new energy and high value-added products.

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ACS Sustainable Chemistry & Engineering · 2025 · IF 7.3

High-Entropy Doped Ni-Rich Oxide Cathodes with Alleviated H2–H3 Phase Transition for Li-Ion and All-Solid-State Li Batteries

Maosheng Gong,Yadong Wei,Hongzhou Zhang,Jingyuan Liu,Xin Zhang,Xuanming Chang,Peiyu Hou,Xijin Xu,Lianqi Zhang

High-capacity Ni-rich cathodes hold considerable promise in advancing both high-energy Li-ion batteries (LIBs) and all-solid-state Li batteries (ASSLBs). Yet, lattice volume changes induced by the H2–H3 phase transition lead to structural degradation. It has been demonstrated that doping approaches can enhance structural stability. Nevertheless, the selection of an appropriate dopant is of considerable importance for the design of high-performance Ni-rich materials with high-entropy doping. Furthermore, the feasibility of high-entropy doped Ni-rich cathodes in ASSLBs has not been reported to date. In this study, leveraging the chemically competitive doping mechanism of Mg, Al, Ti, Nb, and Mo elements, we propose a high-entropy doped LiNi0.8Co0.1Mn0.05Mg0.01Al0.01Ti0.01Nb0.01Mo0.01O2 (HE-NCM) to stabilize Ni-rich cathodes. In-situ X-ray diffraction confirms that the synergistic effect of multiple dopants in high-entropy doping significantly alleviates the H2–H3 phase transition and reduces lattice volume changes, which contribute to the absence of microcracks and improved bulk/interface stability. In ASSLBs, the HE-NCM@LiNbO3 maintains an outstanding capacity retention of 84.5% even after 1700 cycles, demonstrating the feasibility of high-entropy doped Ni-rich cathodes when matched with a sulfide solid-state electrolyte. The application of high-entropy doping methodology for the development of advanced rechargeable batteries has been shown to provide a novel perspective on the improvement of the structural robustness and interfacial compatibility of Ni-rich cathode materials.

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Journal of Materials Chemistry A · 2025 · IF 9.5

Surface-tension-free fabrication to minimize defects in cobalt-silica membranes via the freeze-drying technique for H2 separation at high temperatures

Tanzila Anjum,Hammad Saulat,Gianni Olguin,David K. Wang,Xiaozhen Zhang,Xiaonan Kou,Xian Yin,Asim Laeeq Khan,Guozhao Ji

Hydrogen is a promising substitute for fossil fuels because it has a high calorific value and is eco-friendly. Cobalt-doped silica membranes, suitable for separating hydrogen from other larger molecular gases at high temperatures, are commonly fabricated by the dip-coating method, followed by evaporation drying and calcination. However, these membranes suffer from defects within selective layers, reducing the separation efficiency by allowing non-selective permeation. These defects can be ascribed to surface tension effects during evaporation drying, where the imbalance between liquid-phase cohesion and adhesive interactions with the solid substrate leads to non-uniform solvent evaporation, resulting in stress accumulation, capillary forces, and eventual structural imperfections such as cracks and pinholes. In this study, a novel freeze-drying technique is introduced to minimize defects in cobalt-silica membranes by avoiding surface tension. For this purpose, α-alumina substrates were selected, and a zeolite interlayer was formed on the substrate, which provided the pore size transition to fabricate cobalt-doped silica separation membranes. The structural and morphological analyses confirm the effectiveness of the freeze-drying technique, revealing a higher silica condensation, increased amorphous character, smoother surfaces, homogeneous cobalt dispersion with the presence of Co3+, and uniform, smaller pore sizes, outperforming the evaporation-dried technique in terms of separation efficiency and indicating fewer defects. At 500 °C, the freeze-dried membrane showed almost three times higher H2/N2 and H2/CO2 selectivity than the conventional evaporation-dried membrane. The novel freeze-drying technique showed a promising potential for H2 separation applications at high temperatures.

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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Self-assembly of structured CeCO3OH and its decomposition in H2 for a novel tactic to obtain CeO2-x with excellent photocatalytic property

Xisong Mao,Xuewen Xia,Junqi Li,Chaoyi Chen,Xiaoying Gu,Song Li,Yuan-Pei Lan

In this work, various new-observed structured CeCO 3 OH were synthesized by a self-assembly hydrothermal method , and a novel tactic to produce CeO 2- x with excellent photocatalytic activity by decomposing CeCO 3 OH in H 2 was proposed and identified. By controlling the synthetic conditions, almond-like, subglobose shape and hollow-sphere of CeCO 3 OH, 3D-broom-like of Ce 2 O 3 · 2CO 2 · nH 2 O (n = (1–2)), and sheet-like of Ce 2 (CO 3 ) 3 · 6H 2 O were synthesized. The crystal growth and formation of the cerium carbonate compounds were carefully studied using XRD , SEM and TEM. TG, thermodynamic calculation and in-situ XRD were employed to reveal the decomposition behavior of almond-like CeCO 3 OH in air, Ar and H 2 . The results show that the decomposition temperatures of CeCO 3 OH in Ar and H 2 are higher than that of in air, and suggest that Ce 2 O 3 has a low thermodynamic stability during the decomposition of CeCO 3 OH in Ar and H 2 , and Ce 3+ will be mostly oxidized by H 2 O firstly and then by both of H 2 O and CO 2 . The ceria samples obtained by decomposing from CeCO 3 OH in different atmosphere maintain indistinguishable shape and particle size. The XPS , Raman spectra and ESR results indicate that the one obtained in H 2 has the richest surface oxygen vacancies (OVs), narrowest band gap of 3.12 eV, lowest intensity in PL spectra and a significantly enhanced photodegradation ratio of methylene blue. The MB photodegradation ratio after 120 min reaction with the catalysts of CeO 2 -Air, CeO 2 -Ar and CeO 2 -H 2 is 43.14%, 54.43% and 73.41%, with a calculated reaction rate constant of 0.00539, 0.00652 and 0.01097 min -1 , respectively. The offered novel tactic of decomposing CeCO 3 OH in H 2 is an efficient and facile technique for active CeO 2- x production.

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ACS Omega · 2021 · IF 3.512

Synergistic Effect of Ni/W/Cu on MgAl2O4 for One-Pot Hydrogenolysis of Cellulose to Ethylene Glycol at a Low H2 Pressure

Jun Yu,Jiezhen Liang,Xiaopeng Chen,Linlin Wang,Xiaojie Wei,Youqi Li,Yanmin Qin

Nickel and tungsten, combined with copper, were incorporated into a magnesium aluminum spinel to form a multifunctional catalyst (Ni–W–Cu/MgAl2O4). Characterization results suggested that the adjacent Cu not only facilitated the reduction of W6+ to W5+ with substantial oxygen vacancies but also promoted the reducibility of the Ni species. Besides, the incorporation of Ni, W, and Cu into the support enhanced the catalytic acidity, as well as the L acid sites. The catalyst exhibited a strong synergistic effect between the three metals and the support, resulting in higher catalytic activity for the one-pot hydrogenolysis of cellulose to ethylene glycol. High cellulose conversion (100%) and ethylene glycol yield (52.8%) were obtained, even under a low H2 pressure of 3 MPa.

✓ 已验证 DOI PubMed 高影响因子
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2022 ·Vol. 29 ·期 23 ·34861-34873 · IF 5.19

Vertically grown CeO2 and TiO2 nanoparticles over the MIL53Fe MOF as proper band alignments for efficient H2 generation and 2,4-DCP degradation

Humayun Muhammad,Shu Lang,Pi Wenbo,Xia Hui,Khan Abbas,Zheng Zhiping,Fu Qiuyun,Tian Yahui,Luo Wei

The design of highly efficient photoca talysts for clean energy production and environmental remediation are the grand challenges of scientific research. Herein, TiO 2 @MIL53Fe and CeO 2 @MIL53Fe composite photocatalysts are synthesized via solvothermal technique. The SEM and TEM micrographs reveal that TiO 2 and CeO 2 nanoparticles are vertically grown onto the surface of MIL53Fe MOF. Further, HRTEM micrograph confirmed the formation of heterojunction. It has been investigated that the resultant TiO 2 @MIL53Fe and CeO 2 @MIL53Fe photocatalysts exhibit remarkably improved visible light activities for H 2 production and 2,4-dichlorophenol (2,4-DCP) degradation in comparison to the bare MIL53Fe photocatalyst. The enhanced photoactivities of the fabricated TiO 2 @MIL53Fe and CeO 2 @MIL53Fe photocatalysts are attributed to significantly promoted charge separation as confirmed via the surface photo voltage (SPV) and photoluminescence (PL) results. Further, the photocatalysts exhibit high stability and reusability as confirmed via the recyclable tests. This work will promote the design of MOF-based efficient photocatalysts for clean energy production and environment purification.

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ADVANCED FUNCTIONAL MATERIALS · 2026 · IF 19.9

Fine-Tuning Sub-Ångström Pores in Carbon Molecular Sieve Membranes via UV-Crosslinking Induced Super-Network Polyimide Precursors for Ultra-Selective H2 Purification

Mingwei Cai,Fuhui Liang,Huahui Liang,Congcong Wu,Luxin Sun,Xiaohua Ma,Shiyang Zhang,Yonggang Min

Achieving precise customization and structural regulation of sub-Ångström pores of Carbon molecular sieve membranes (CMSMs) remains challenging. In this study, CMSMs with ultra-high H 2 /CH 4 separation performance were developed by a UV induced super-crosslinking network polyimide precursor, which was formed by click reaction through an imide intermediate that contains C≡CH and the SH as functional end groups. The as-formed polyimide contains C═C─S in each repeat unit of the polyimide which can be crosslinked using UV light via the [2+2] reaction and form molecular “stitches” with a super-crosslinking network. The cross-linking node density can be easily adjusted by the UV irradiation time (0–30 min). During pyrolysis, the dimensions of the connecting interior pore necks for sub-Ångström pores can be fine-tuned (4.0±0.3 Å), promoting the formation of a higher concentrated (4%–8%) sub-4 Å pores. The optimized CMS-30 membrane demonstrates outstanding gas separation performance, with H 2 permeability of 2930 Barrer and remarkable selectivity for H 2 /CH 4 (4651), surpassing the Robeson upper bounds and outperforming most reported CMSMs. This photo-induced super-crosslinking network precursor method provides a versatile strategy for high-performance CMSM by sub-nanometer precision engineering of CMSMs.

CAS / MDL: 1107-00-2 1193-02-8
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JOURNAL OF ALLOYS AND COMPOUNDS · 2026 · IF 6.7

The CdS/CuS heterojunction prepared by room-temperature vulcanization of Cu-BTC accelerates charge carrier transfer to achieving high-efficiency photocatalytic H2 evolution

Ning Qi,Hongchao Qi,Tianrong Xiong,Youzhou He,Qinghong Cai,Zhuoqi Liu,Panyin Wang,Yongcheng Feng,Lin Chen,Bowen Lei,Xingyan Liu

The interfacial agglomeration in photocatalysts synthesized via high-temperature methods leads to hindered charge carrier mobility, severely limiting their photocatalytic performance. Herein, we introduced a room-temperature sulfidation strategy for the fabrication of CdS/CuS heterojunctions utilizing Cu-BTC. The optimized CdS/CuS composite demonstrated an exceptional hydrogen evolution rate of 14.07 mmol·h −1 ·g −1 , which was 7.5 times greater than that of pristine CdS. The slow release of Cu 2+ from Cu-BTC at room temperature effectively inhibited interfacial agglomeration. This was further confirmed by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Furthermore, the formation of a CdS/CuS type-II heterojunction was confirmed by Mott-Schottky measurements, Tauc analysis, and valence band X-ray photoelectron spectroscopy (VB-XPS) analysis. Owing to the interfacial electronic coupling of CdS/CuS, charge carrier recombination is suppressed while carrier migration and separation are accelerated, leading to a significant enhancement in the hydrogen evolution activity. This work therefore proposes a feasible room-temperature synthesis strategy for fabricating high-quality heterojunctions, which effectively suppresses interfacial agglomeration and accelerates charge carrier transfer, resulting in enhanced photocatalytic performance.

CAS / MDL: 68-12-2
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FLUID PHASE EQUILIBRIA · 2026 · IF 2.7

High-temperature solubility and thermodynamic correlation of CO2, H2, and CH4 in 1-Ethyl-2-pyrrolidone: Implications for catalytic CO2 hydrogenation to ethanol

Yufan Ma,Cong Liu,Hongxing Wang,Jie Li,Qingli Qian

The solubilities of CO 2 , H 2 , and CH 4 in 1-ethyl-2-pyrrolidone (NEP) were measured using the isochoric saturation method at 413.15–453.15 K under pressures of 0.45–3.89 MPa (CO 2 ), 4.42–7.64 MPa (H 2 ), and 0.59–3.49 MPa (CH 4 ). The reliability of the apparatus was verified by measuring CO 2 solubility in N-methyl-2-pyrrolidone (NMP) at 323.15–353.15 K. The solubility order in NEP was found to be CO 2 > CH 4 > H 2 . Temperature-dependent Henry’s constants were obtained, and the experimental data were correlated using the Krichevsky–Kasarnovsky equation and the generic Redlich–Kwong (RK) cubic equation of state, with the RK model providing better accuracy. These results offer essential thermodynamic data for describing gas–liquid equilibrium in NEP and support solvent selection and process design in high-temperature CO 2 conversion systems.

CAS / MDL: 872-50-4
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Nanoscale · 2022 ·Vol. 14 ·期 42 ·15889-15896 · IF 8.307

In situ Cu single atoms anchoring on MOF-derived porous TiO2 for the efficient separation of photon-generated carriers and photocatalytic H2 evolution

Yuxiang Ma,Yumin Zhang,Yiwen Ma,Tianping Lv,Bin Xiao,Xinya Kuang,Xiyu Deng,Jin Zhang,Jianhong Zhao,Qingju Liu

Single atom catalysts (SACs) have an extremely high atom utilization and distinctive structures and properties in the field of photocatalysis. However, the premise of conducting scientific research and applications is still the stability and catalytic activity of single atoms on suitable substrates. Metal organic frameworks (MOFs), as one of the most suitable single-atom substrates, have tunable internal structures, unsaturated coordination bonds, and high specific surface areas. In this work, Ti-based MOF, MIL-125, was adopted as the precursor to prepare mesoporous Cu-loaded TiO2. During the synthesis of MIL-125, a Cu source was added, and Cu atoms were fixed by partly replacing Ti atoms in the Ti–O octahedron to coordinate with O atoms, resulting in a good dispersity, good stability and high loading amount. Experimental investigations demonstrated that dispersed Cu single atoms act as reaction centres, besides being able to accelerate the transfer of photoelectrons. Under simulated sunlight, the H2 evolution rate of the optimum Cu–TiO2 sample reaches 17.77 mmol g−1 h−1, nearly 101 times higher than that of the pure mesoporous TiO2. The apparent quantum efficiency (AQE) is 20.15% under 365 nm irradiation. This research opens a new thinking to preparing high stability and high activity single atom photocatalysts.

研究领域: 材料科学 · 光催化 · 能源科学
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