JOURNAL OF CATALYSIS
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2026
·
IF 6
Xu Chen,Weijing Cao,Ziyi Fan,En Zhao,Lang Zhou,Zupeng Chen
AuPd-TCN enables photocatalytic 5-HMF oxidation coupled with H 2 evolution. • Achieving 69.2% DFF yield and 421.9 μmol·g⁻ 1 ·h⁻ 1 H 2 evolution rate within 2 h. • Revealing AuPd-TCN interfacial interactions to promote charge separation and transfer. • Confirming valence-band oxidation and conduction-band reduction coupling by DRIFTS and EPR. The selective oxidation of 5-hydroxymethylfurfural (5-HMF) to 2,5-diformylfuran (DFF) coupled with hydrogen (H 2 ) evolution offers a sustainable strategy for the high-value conversion of biomass-derived platform chemicals and clean energy production. In this study, tubular carbon nitride (TCN) is first prepared via self-assemble of a supramolecular precursor, followed by the loading of AuPd bimetallic nanoparticles on its surface through an impregnation-reduction method to construct the AuPd-TCN photocatalyst. Under visible-light irradiation for 2 h, AuPd-TCN delivers a DFF yield of 69.2% and a H 2 evolution rate of 421.9 μmol·g −1 ·h −1 , markedly outperforming pristine TCN (22.4%, 17.7 μmol·g −1 ·h −1 ), Au-TCN (39.8%, 204.2 μmol·g −1 ·h −1 ), and Pd-TCN (48.6%, 255.4 μmol·g −1 ·h −1 ). Structural and photoelectrochemical characterizations reveal that Au and Pd form bimetallic nanoparticles on TCN with strong interfacial electronic interactions that promote the separation and transfer of photogenerated charge carriers. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) confirms that the hydroxymethyl group of 5-HMF is selectively oxidized to an aldehyde group, while the furan ring skeleton remains intact during the reaction. Active species trapping experiments and electron paramagnetic resonance (EPR) analysis further demonstrate that photogenerated holes (h + ) and electrons (e - ) are the primary active species in this coupled reaction: h⁺ drives the selective oxidation of 5-HMF to DFF, while e - reduces H⁺ to H 2 on the AuPd bimetallic nanoparticles surface. This study provides an effective strategy for simultaneous biomass-derived chemical valorization and clean hydrogen production. Download: Download high-res image (147KB) Download: Download full-size image
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Hong Tian,Jiwen Fu,Lei Liu,Hongyu Chen,Zheng Zeng,Sijin Chen,Fubin Ma
With moderate N content and rich micropore, NC-AC shows the highest CO 2 uptake. • N-doping and pore structure control low/high-pressure CO 2 sorption, respectively. • Optimal pore size for CO 2 adsorption increases with adsorption pressure. • Pyrrolic N exhibits the most significant enhancement in CO 2 adsorption. In steam methane reforming (SMR) for hydrogen production, efficient CO 2 removal is essential. Although ultra-micropores and nitrogen doping enhance CO 2 adsorption on carbon adsorbents, their combined effects under high-pressure conditions remain unclear. Herein, a nitrogen-doped biochar (NC), an activated biochar (AC), and a nitrogen-doped activated carbon (NC-AC) were prepared from waste coconut shell. AC exhibited a highly developed pore structure (specific surface area of 1755 m 2 /g and micropore volume of 0.644 cm 3 /g), whereas NC was rich in nitrogen content (16.49 wt%). NC-AC combined a moderate nitrogen content (3.06 wt%) with an abundant porous network. High-pressure CO 2 adsorption isotherms revealed a pressure-dependent evolution in the relative contributions of nitrogen-containing functional groups and pore structure: the contribution of nitrogen-containing functional groups was more pronounced at low pressures (<0.5 bar), the contribution of pore structure gradually increased at intermediate pressures (0.5–2 bar), and pore structure played a more pronounced role at high pressures (>2 bar). Dynamic column breakthrough experiments with a CO 2 /H 2 mixture (20/80 vol%) demonstrated that NC-AC exhibited the highest CO 2 uptake. Molecular simulations showed that at low pressure, the 0.6 nm pore exhibited the highest CO 2 adsorption, while at 10 bar, the 0.8 nm pore surpassed due to its strong interaction forces and large packing space. In the 0.8–1.0 nm pores, CO 2 preferentially formed multilayer adsorption near the pore walls and pushed H 2 toward the pore center. Among nitrogen-functional groups, pyrrolic N (N-5) significantly enhanced the CO 2 adsorption capacity and selectivity. Download: Download high-res image (94KB) Download: Download full-size image
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ACS Applied Nano Materials
·
2026
·
IF 5.8
Cui Zhiqing,Wu Hao,Li Mingyue,Lv Liwei,Chen Huamao,Huang Jiawang,Li Taotao,Hu Jinwu,Fang Caihong
Exploration of efficient and nonprecious electrocatalysts
is essential
to propel water electrolysis toward developing a sustainable world.
Herein, we demonstrated heterogeneous Ni–NiWO 4 nanostructures
grown in situ on nickel foam (NF) (Ni–NiWO 4 /NF),
serving as effective bifunctional electrocatalysts toward the hydrogen
evolution reaction (HER) and urea oxidation reaction (UOR), enabling
high-performance overall urea splitting reaction (OUS) in both freshwater
and seawater. The favorable porous architecture provides a large electrochemically
active surface area and facilitates mass transfer. The coupling between
Ni nanoparticles and the NiWO 4 matrix creates an electron-rich
microenvironment and modulates the electronic states of the active
sites, which provides optimal chemical affinities for various reaction
intermediates, as confirmed by our calculation through density functional
theory calculations. Specifically, the Ni–NiWO 4 /NF
electrocatalyst exhibits low overpotentials of 26 mV@10 mA cm –2 , 126 mV@100 mA cm –2 , and 156 mV@200
mA cm –2 in alkaline freshwater and 31 mV@10 mA cm –2 , 162 mV@100 mA cm –2 , and 212 mV@200
mA cm –2 in alkaline seawater for the HER. Remarkably,
the overpotential is as low as 265 mV, even when the current density
was evaluated to be as high as 1.0 A cm –2 . For the
UOR, it demonstrates low potentials of 1.292 V@10 mA cm –2 , 1.343 V@100 mA cm –2 , and 1.374 V@200 mA cm –2 in alkaline freshwater and 1.307 V@10 mA cm –2 , 1.358 V@100 mA cm –2 , and 1.387 V@200 mA cm –2 in alkaline seawater. Notably, the recorded voltage
for the OUS reaction decreases to 1.366 V in freshwater and 1.390
V in seawater. Additionally, the catalyst demonstrates excellent long-term
stability in seawater for 100 h at 10 mA cm –2 . Furthermore,
we successfully demonstrated solar-powered green hydrogen production
at a rate exceeding 510 L h –1 m –2 , showcasing its strong potential for the practical application of
direct solar-to-hydrogen conversion.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Weizhen Xie,Yue Tang,Jiacheng Li,Yaqi Shi,Shigang Su,Yong Sun,Lu Lin,Xing Tang
The aqueous-phase hydrogenation of concentrated 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) is a crucial transformation for sustainable chemical production. However, this process is often limited by sluggish H 2 activation at low temperatures and poor selectivity arising from over-hydrogenation. Here, we develop a Pt catalyst supported on oxygen-deficient manganese oxide (Pt/MnO x –O v ), featuring finely dispersed Pt/PtO 2 domains in conjunction with abundant Pt–O–Mn interfacial ensembles. Under mild aqueous conditions (30–60 °C), the catalyst efficiently converts HMF at concentrations up to 40 wt%, delivering a BHMF yield of 90.9 %. In addition, continuous-flow operation at 30 °C sustains BHMF yields above 90 % over a cumulative operation time of 80 h, thereby demonstrating promising potential for industrial application. Mechanistic studies suggest that hydrogen is initially activated on Pt nanoparticles and subsequently undergoes in situ spillover, migrating across the Pt/PtO 2 heterostructure toward adjacent Pt–O–Mn interfacial sites. At these interfacial regions, the asymmetric electronic distribution, induced by nearby oxygen vacancies, facilitates the formation of polarized H δ+ –H δ- species. These reactive hydrogen species, together with the preferential adsorption of the carbonyl group, enable selective hydrogenation while suppressing undesired side reactions. This study demonstrates that tailoring interfacial structures is an effective strategy for improving catalytic performance in biomass upgrading.
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BIOMATERIALS
·
2026
·
IF 13.6
Zishuo Hou,Yue Yuan,Gangfeng Li,Haowei Peng,Jiena Weng,Hongbo Wei,Tengjiao Wang,Peng Li
Soft tissue integration around implants is severely compromised by the inflammatory microenvironment, often leading to implant failure. However, due to the bioinert nature of titanium (Ti), effective strategies to regulate this microenvironment remain limited. Herein, we propose a poly(lipoic acid)-based antibacterial polymer (pLAP) enabling controlled molecular hydrogen (H 2 ) release to achieve both antibacterial and pro-regenerative effects for this critical challenge. The pLAP exhibits potent antibacterial activity, achieving killing efficiencies of 90.71% and 94.62% against Staphylococcus aureus and Porphyromonas gingivalis , respectively. Notably, the strong adhesion of pLAP to substrate and its affinity for bacterial membranes contribute to its durable and sustained antibacterial performance. Owing to the encapsulation of H 2 -loaded TiO 2 nanotubes within pLAP and its intrinsic biodegradability, a delayed and sustained H 2 release profile is achieved, with H 2 levels rising to 427 ppb within 24 h and persisting above 300 ppb for at least 72 h. In vitro and in vivo studies demonstrate that released H 2 alleviates oxidative stress and modulates immune responses, with suppression of the JAK1-STAT1 and activation of the JAK3-STAT6 signaling pathways associated with these effects, promoting M2 polarization and enhancing soft tissue integration. Collectively, this work presents a robust and generalizable strategy for regulating the inflammatory microenvironment in peri-implantitis and other implant-associated inflammatory conditions.
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ACS Catalysis
·
2026
·
IF 13.6
Shibin Zhang,Xu Sun,Fenghuan Zhao,Zhipeng Xu,Hongyu Zhao,Shikang Zhang,Bohua Dong,Junjie Qin,Lixin Cao,Chenghui Xia
Efficient photocatalytic H2 evolution in natural seawater is challenged by sluggish interfacial electron extraction, severe carrier recombination, and deteriorated surface reaction kinetics in saline media. Here, we construct a CdS−NiCoSx Schottky heterojunction by integrating snowflake-like CdS with an amorphous hollow NiCoSx cocatalyst, where Ni incorporation simultaneously modulates the spin-related electronic structure of the cocatalyst and the interfacial Schottky energetics. Under visible-light irradiation (λ > 420 nm) in the presence of sacrificial reagents, the optimized photocatalyst delivers an H2 evolution rate of 19.89 mmol g−1 h−1 in natural seawater and 29.44 mmol g−1 h−1 in pure water, outperforming pristine CdS by 8.23-fold and an optimized CdS−Pt benchmark by 2.51-fold under identical conditions while retaining 92% of its initial activity after 16 h in natural seawater. Spectroscopic, photoelectrochemical, magnetic, and theoretical analyses collectively indicate that Ni incorporation increases the work function of the cocatalyst, strengthens band bending at the CdS−cocatalyst interface, and enhances the spin asymmetry of electronic states near the Fermi level. These changes facilitate interfacial electron extraction and suppress charge recombination. In parallel, Ni incorporation improves H2O adsorption and moderates H* binding at Co-centered sites, thereby accelerating the intrinsic kinetics of hydrogen evolution. This work identifies Ni incorporation as an effective means of coupling spin-state modulation with Schottky junction engineering in sulfide cocatalysts and provides a more rigorous framework for designing photocatalysts for sacrificial H2 evolution in natural seawater.
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ACS Sensors
·
2026
·
IF 10.9
Leiyu Diao,Ou Wang,Dong Cheng,Qing Yue,Youyou Feng,Yaqiong Su,Jing Wei
Noble-metal catalysts have been widely used for high-performance semiconductor metal oxide hydrogen sensors due to their excellent adsorption and activation capacity for H2 molecules. However, the subsequent redox reaction between activated hydrogen (H*) and oxygen remains challenging due to the limited chemisorbed oxygen species on the surface of the semiconductor metal oxide. Here, we develop PtPd bimetallic nanoparticle-decorated WO3 nanosheets to overcome this bottleneck by coupling hydrogen spillover with reversible W6+/W5+ transformation. Gas-sensing measurements show that PtPd-WO3 gives a response of 298% toward 10 ppm H2 at 150 °C, which is 37.3 and 3.6 times higher than those of pristine WO3 and Pd-WO3, respectively. The response time is reduced to 4 s (15 s for WO3). Mechanism analysis reveals that the bimetal PtPd not only facilitates H2 dissociation but also triggers the “activation” of the WO3 surface. Abundant H* species, bypassing the limitation of chemisorbed oxygen species, permeate into the WO3 lattice to drive reversible W6+ to W5+ reduction. This bulk-involved lattice redox process drastically modulates the resistance of WO3 and amplifies the sensing signals. In situ Raman spectroscopy, gasochromic experiments, and density functional theory calculations substantiate that the PtPd-induced reversible lattice redox process is key to accelerating interfacial reactions. Finally, the PtPd-WO3 sensor was integrated into a wireless platform for unmanned aerial vehicle-based and distributed pipeline monitoring, enabling real-time hydrogen leak localization.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2026
·
IF 6.7
Dexin Kong,Rui Shan,Shuxiao Wang,Huan Li,Haoran Yuan,Yong Chen
Converting plastic waste into hydrogen provides a promising route to simultaneously address environmental pollution and clean energy production. This study developed a Ni single-atom catalyst stabilized on an Al 2 O 3 /N-C composite support (Ni@Al 2 O 3 /N-C) for H 2 production from polypropylene (PP) via pyrolysis-catalytic reforming. The composite support integrates the high-temperature structural stability of Al 2 O 3 with the strong anchoring capability of N-doped carbon, enabling the formation of stable C-N-Ni active sites and effectively suppressing Ni aggregation under harsh reforming conditions. Under the optimal conditions (catalyst/PP = 1.25:1, water feed = 6 mL h −1 ), the catalyst achieved a gas yield of 127.59 mmol g −1 PP, a hydrogen yield of 84.14 mmol g −1 PP, and a hydrogen selectivity of 65.96%. The catalyst maintained good cyclic performance over 10 consecutive runs, with the H 2 yield decreasing from 84.14 to 69.39 mmol g −1 PP while the H 2 selectivity remained at 64.49% in the 10th cycle. XPS, HAADF-STEM, XRD, Raman, SEM, and TEM analyses confirmed that Ni remained atomically dispersed on the support after reaction, with no obvious nanoparticle agglomeration and only limited carbon nanotube formation. This work provides an effective support-engineering strategy for designing thermally stable single-atom catalysts for plastic reforming and other high-temperature catalytic processes.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Zecheng Lv,Enjun Zhu,Lanyun Wang,Yongliang Xu,Yuanwei Huang,Kun Zhang,Xiaodong Feng
H 2 + CH 4 hydrate is a promising solid state gas-storage medium, but its slow formation and limited stability under heating conditions restrict its practical application. In this study, 1,3-dioxolane (1,3-DIOX) and perfluorooctane (C 8 F 18 ) were used as single and combined additives for H 2 + CH 4 hydrate formation with a 25 mol% H 2 + 75 mol% CH 4 gas mixture. Their effects on phase equilibrium, nucleation, gas uptake, and heating-induced dissociation behavior were investigated. 1,3-DIOX acted as the dominant thermodynamic and kinetic promoter, yielding equilibrium temperatures of 291.05–293.75 K at pressures of 4.90–7.02 MPa and producing the highest gas uptake of 0.09781 mol/mol. In contrast, C 8 F 18 had limited influence on phase equilibrium and formation kinetics but delayed gas release during heating-induced dissociation. The combined system showed functional complementarity between formation promotion and dissociation-response regulation for H 2 + CH 4 hydrate storage.
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Advanced Science
·
2026
·
IF 14.1
Zesheng Chen,Yanchao Yu,Xingyuan Xiao,Wenwen Cheng,Ye Yang,Zhengyao Zhang,Wang Wang,Zhijun Zhou,Weikang Hu,Xiaolong Wang,Bing Li,Kwang Leong Choy,Yun Chen,Zijian Wang
Impaired wound healing in diabetes is closely associated with cellular ferroptosis. Microneedle-assisted gas therapy exerts molecular regulation of ferroptosis, representing a promising approach for accelerating diabetic wound healing. To date, O 2 and H 2 gas therapies have consistently been conducted independently and have never been integrated into a single system. Whether and how their synergy might be realized remains a defining challenge. Herein, we propose a concept of integrated O 2 and H 2 gas therapy, demonstrated by fabricating a gas-producing microneedle material. Platinum@MIL-101(Fe)-NH 2 @phosphotungstic acid (PMP) nanoparticles are synthesized as a visible light-driven photocatalyst for H 2 and O 2 co-evolution. The rational design of a spatially separated structure boosts their photocatalytic efficiency under physiological conditions. PMP nanoparticles are further incorporated with bilayer gelatin methacryloyl (GelMA)/PMP composite microneedles (denoted as GPM microneedles). The obtained GPM microneedles enable transdermal delivery of PMP nanoparticles for integrated O 2 and H 2 gas therapy, and demonstrate desirable biocompatibility and pro-regenerative effects. The mechanism of integrated O 2 and H 2 gas therapy has been identified as a TNFAIP3/hnRNPA1 ubiquitination/ferroptosis signaling axis, establishing for the first time a direct link to ferroptosis. In conclusion, this study yields a transformative concept and a ferroptosis-targeting microneedle material with well-defined molecular mechanism for diabetic wound management.
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高影响因子
BIORESOURCE TECHNOLOGY
·
2026
·
IF 8.2
Xumiao Mao,Weiqiang Jiang,Qian Chen,Xiaojun Fan,Hongguang Guo,Jin Yuan,Xin Kong
ZVI boosts straw hydrolysate H 2 yield (24.53%) and H 2 /CO 2 (26.9%) at 55 °C. • ZVI amendment markedly elevates hydrogenase and acetate kinase activities. • ZVI addition reshapes the microbial community into a syntrophic consortium. • ZVI upregulates key genes of acetate-producing pathway in butyrate-type fermentation. Deep strata anaerobic fermentation of crop straw hydrolysate for bio-hydrogen (H 2 ) production mitigates open-field burning pollution and supports net-negative carbon emissions by substituting and converting geologically sequestered CO 2 into CH 4 . However, the thermophilic conditions in deep strata differ significantly from traditional mesophilic systems for biohydrogen fermentation. Crucially, optimizing subsequent methanogenesis of pre-stored CO 2 requires enhancing H 2 yield and H 2 /CO 2 ratio simultaneously. This study demonstrates that zero-valent iron (ZVI) can enhance the biohydrogen during straw hydrolysate fermentation at 55 °C. Experimental results indicate that, compared to the control, the reactor with a ZVI dosage of 1 g/L exhibited a 24.53% increase in cumulative hydrogen yield, accompanied by a 26.90% elevation in the H 2 /CO 2 ratio, thereby achieving simultaneous improvements in both hydrogen yield and purity. Mechanistic investigation reveal that ZVI maintains appropriate reductive conditions and faciliates interspecies electron transfer efficiency within the fermentation system. Moreover, molecular ecological network analysis indicates that ZVI promotes the formation of syntrophic microbial networks. KEGG-based functional predictions further suggest that key enzyme genes associated with glycolysis and butyrate-type fermentation were upregulated, whereas the expression of genes participating in non-hydrogen-producing pathways was suppressed. Furthermore, acetyl-CoA metabolism was shifted toward the acetate pathway during butyrate-type fermentation, favoring elevated hydrogen production while suppressing CO 2 co-generation. This study establishes a conceptual and experimental foundation for achieving net-negative carbon emissions via straw-derived biohydrogen in deep strata, although significant engineering challenges remain. Download: Download high-res image (198KB) Download: Download full-size image
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Shikai Wang,Dafeng Zhang,Ping Su,Xintong Yao,Junchang Liu,Xipeng Pu,Hengshuai Li,Peiqing Cai
The reasonable design and fabrication of heterojunction could regulate the photocatalytic performance to some extent, yet it is still a great challenge to construct the S-scheme heterostructure with the stable as well as tight interface on the surface of semiconductor photocatalysts. Herein, the ZnIn 2 S 4 /Cu 2 MoS 4 (ZIS/CMS) S-scheme heterostructure was fabricated by in-situ assembling ZIS nanosheets on the CMS plates, obtaining a mossy tile-like morphology. Owing to the compact interface resulting from in-situ growth, this unique architecture efficiently facilitated the separation and transfer of light-induced charges, guaranteed the larger interface area, and enriched the active sites for photocatalytic redox reactions. After adjusting the mass ratio of CMS in ZIS/CMS, S-scheme heterostructure exhibited the remarkable performance with an optimal H 2 producing rate up to 1298 μmol·h −1 g −1 , about 13.8 times than that of pristine ZIS. The mechanism and driving force of charge transfer and separation in S-scheme heterostructure photocatalysts were explained and discussed. This investigation will provide new insight into design and construction of S-scheme heterojunction photocatalysts for H 2 evolution.
研究领域:
材料科学
·
能源化学
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