CARBON
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2022
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IF 11.307
Lizhen Hu,Teng Wang,Qianqian Nie,Jiayou Liu,Yunpei Cui,Kefei Zhang,Zhongchao Tan,Hesheng Yu
Efficient, stable, and selective photocatalytic conversion of nitric oxide (NO) into nitrogen dioxide (NO 2 ) is highly desirable but remains a big challenge. We prepare single atom catalyst (SAC) by anchoring single Pd atoms onto graphitic carbon nitride (CNPd) via chemical impregnation followed by calcination . The prepared CNPd SAC is confirmed by aberration-correction high-angle-annular-dark field scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy. The synthesized SAC outperforms its competitors reported earlier for photocatalytic removal of NO under visible light and simulated sunlight irradiation in terms of selectivity and stability. The SAC maintains a NO removal efficiency of 83% and an instantaneous selectivity for NO 2 of 92.8% over 117.6 h under simulated sunlight with the inlet NO concentration of 12 ppm. This duration is about 23.5 times the longest duration tested for other catalysts in the literature. The experimental results and density functional theory (DFT) calculations reveal that single Pd atom promotes the photocatalytic degradation of NO. Moreover, the DFT calculations prove that the nitrate ions that accumulate on the surface of the SAC can react with NO to produce NO 2 . This reaction enhances the selectivity for NO 2 and stability of the SAC.
研究领域:
环境科学
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材料科学
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化学
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Liangmin Xiong,Shuang Liu,Yong Men,Lin Li,Xiaoda Niu,Kailiang Guo,Junzhe Xu,Wei An,Jinguo Wang,Yu Cong
CO 2 hydrogenation to liquid fuels is significant to reduce CO 2 emissions and replace fossil fuels . Herein, we reported that Fe catalysts promoted by combination of K and Pd showed a three-synergistic catalytic effect to high selectivity of C 5+ hydrocarbons in CO 2 hydrogenation reaction. The catalysts were prepared using an impregnation method and characterized with physical adsorption , XRD , XPS , HRTEM , H 2 -TPR, H 2 -TPD and CO 2 -TPD. The results indicated that K 0.016 Pd 0.12 Fe catalysts showed K-overlapped PdFe-like alloy structure which enhanced H 2 activation behaviors and moderately chemisorption of CO 2 . K addition promoted Fe to activate carbide species while active H originated from H 2 pool generated by PdFe alloy spilled to Fe species surface, consequently boosting not only conversion of CO 2 to 41.8% but also selectivity of C 5+ hydrocarbon to 70.6%. The maximum yield of long-chain C 5+ hydrocarbon reached up to 20.0% under high space velocity 6000 mL g cat −1 h −1 . These results provide a new insight to develop highly selective Fe based catalysts for long-chain hydrocarbons via CO 2 hydrogenation.
研究领域:
化学工程
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催化反应
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能源转化
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Catalysis Science & Technology
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2021
·Vol. 11
·期 20
·6732-6741
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IF 6.119
Yafeng Chen,Guimin Jiang,Xiangzhi Cui,Zuotai Zhang,Xinmei Hou
Eliminating indoor formaldehyde (HCHO) pollution at room temperature is highly needed to improve the environment while saving energy. Herein, Pd/CeO2 catalysts with different morphologies of the CeO2 support were employed to investigate their performance for HCHO oxidation. The Pd/CeO2 nanocube (Pd/CeO2-C) catalyst exhibited excellent catalytic activity compared to commercial CeO2 and CeO2 nanorods. HCHO can be completely converted into CO2 and H2O over the Pd/CeO2-C (0.64 wt% Pd) catalyst at a weight hourly space velocity of 36 000 mL g−1 h−1 at room temperature. Multiple characterization results confirmed that the strong interfacial interaction between Pd and the CeO2-C support guarantees a high percentage of metallic Pd on the CeO2-C surface and its high dispersion, which is crucial for the oxidation of formaldehyde at low temperature. The in situ diffuse reflectance infrared Fourier transform results indicated that CO, formate and dioxymethylene species are the main intermediates over the Pd/CeO2-C catalyst, and the active O species is responsible for their decomposition and oxidation. This work may promote the practical application of high performance Pd-based catalysts for indoor HCHO purification and related catalytic processes.
研究领域:
环境科学
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催化化学
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Molecular Catalysis
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2024
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IF 3.9
Yu Chen,Ming-Yu Qi,Zi-Rong Tang
Integrating selective organic transformation and hydrogen (H 2 ) evolution in one photoredox reaction system is one of the most sustainable and promising approaches to efficiently produce solar fuels and chemicals by simultaneously utilizing photogenerated electrons and holes. Herein, through the cation-exchange engineering method, the nanoleaf-like Pd/CdS composites are gingerly fabricated for visible-light-driven receptor-free dehydrogenation of 1,2,3,4-tetrahydroisoquinoline (THIQ) to 3,4-dihydroisoquinoline (DHIQ) and H 2 under ambient conditions. The optimized electronic structure endows Pd/CdS with a narrow band gap and suitable energy band positions, thus facilitating the light harvesting as well as the separation and transfer of photoexcited charge carriers. Consequently, the Pd/CdS exhibits significantly improved photoredox activity compared to bare CdS . In-situ Fourier-transform infrared spectroscopy and electron paramagnetic resonance spectroscopy track the progression of reaction intermediates during such a dual-functional photoredox-catalyzed system, revealing that the carbon-centered radical is the key reaction intermediate in this reaction process. It is anticipated that this work would guide the rational utilization of CdS-based materials to enable simultaneous photochemical coupling of organic transformation and H 2 evolution.
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SENSORS AND ACTUATORS A-PHYSICAL
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2026
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IF 5.1
Peicheng Han,Yunbo Shi,Canda Zheng,Bolun Tang,Qiaohua Feng
Green hydrothermal synthesis of flower-like WSe 2 using biodegradable ascorbic acid as the reducing agent. • Vacuum sintering at 450 ∘ C improved the crystallinity, surface activity, and charge transport of WSe 2 enhancing NO 2 sensing. • Optimal 3% Pd decoration enabled catalytic/interfacial sensitization, achieving a response of 2.26 toward 16 ppm NO 2 with good selectivity and stability. Although WSe 2 has shown great potential for NO 2 sensing, its development remains challenging because conventional hydrothermal synthesis often relies on hazardous reducing agents such as NaBH 4 and N 2 H 4 ⋅ H 2 O, which may cause rapid H 2 release, toxicity, and environmentally harmful byproducts. In addition, the sensing performance of WSe 2 is often limited by insufficient active sites and inefficient charge transfer. Herein, flower-like WSe 2 nanostructures were synthesized via a one-step hydrothermal route using benign, biodegradable, eco-friendly, and cost-effective C 6 H 8 O 6 as the reducing agent. The obtained WSe 2 was vacuum-sintered at the optimized temperature of 450 ∘ C and further decorated with Pd nanoparticles to enhance NO 2 sensing performance. The optimized 3% Pd-WSe 2 -450 ∘ C sensor exhibited a response ( R a / R g ) of 2.26 toward 16 ppm NO 2 at an operating temperature of 114 ∘ C, with response and recovery times of 20 and 190 s, respectively. The enhanced sensing performance is attributed to the synergistic effects of Pd decoration, improved crystallinity, abundant surface oxygen species, and efficient interfacial charge modulation. This work demonstrates a Pd-modified WSe 2 -based NO 2 gas sensor, where green synthesis, vacuum sintering, and interfacial Pd engineering synergistically enhance the sensing performance. Download: Download high-res image (368KB) Download: Download full-size image
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ANALYTICA CHIMICA ACTA
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2026
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IF 6.1
Hui-ting Hu,Xiao-mei Li,Wen-cai Jiang,Chen Ni,Yu-yang He,Guo-qi Zhang,Hao Yu,Zhi-Bo Hou
Per- and polyfluoroalkyl substances (PFAS) were a class of hazardous contaminants known for their high environmental persistence and toxicity. Due to their strong polarity, wide variety, and broad distribution, a rapid, accurate, and on-site detection method was urgently needed for future screening and emergency response. Herein, a dandelion-like Pd/Cu nanozyme with triple enzyme-like activities (oxidase-like, peroxidase-like, and laccase-like) was synthesized by one-step hydrothermal method. Different PFAS species inhibited these three enzyme-like activities to varying extents. By quantifying absorbance changes, distinct fingerprint patterns were constructed, and a three-channel colorimetric sensor array was developed. This array exhibited high selectivity and robust anti-interference capability for discriminating seven PFAS species. The LDA score plot revealed distinct clustering of different PFAS classes and complex mixtures, indicating clear separability among their fingerprints. The developed nanozyme sensor array was successfully applied to the detection of PFAS in environmental water (river, lake, and tap water). This work provided a novel strategy for selective and reliable detection of PFAS in complex environmental matrices.
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SENSORS AND ACTUATORS B-CHEMICAL
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2026
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IF 8.3
Xudong Liang,Yuchen Duan,Xiangyu Li,Fujia Zhao,Yunwei Li,Yiming Jian,Lei Shi,Jiayu Li,Guo-Dong Li
Detection of 3-hydroxy-2-butanone (acetoin), a characteristic volatile metabolite of Listeria monocytogenes (LM) , represents a promising non-invasive strategy for monitoring contamination levels of foodborne pathogens in food. However, current sensing materials suffer from poor selectivity and insufficient sensitivity at trace concentrations. Herein, a series of Pd-loaded Cd 2 GeO 4 (Pd/CGO) chemiresistive gas sensors that achieves highly selective and sensitive acetoin detection was reported. Among them, the 0.5 wt% Pd/CGO-based sensor exhibits a high response, with an ultrafast response time and a detection limit as low as 10 ppb. The sensor also demonstrates excellent selectivity over common interfering gases, good reproducibility, and robust long-term stability. Mechanistic investigations combining O 2 -TPD, XPS, and DFT calculations reveal that Pd loading not only increases the proportion of chemisorbed oxygen species on the CGO surface, which enhances the overall sensing response, but also serves as new active sites. This work demonstrates that rational Pd modification combined with dual-site engineering offers a promising paradigm for designing high-performance metal oxide gas sensors for pathogen biomarker detection in food.
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Journal of Energy Chemistry
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2026
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IF 15.6
Mudong Tu,Wenhan Dai,JunFeng Huang,Zhe Zhao,Yantao Wang,Yahan Fang,Lanjuan Yao,Hua Li,Baodui Wang
The efficient utilization of active hydrogen (*H) in electrocatalytic processes remains a critical challenge for achieving high selectivity in nitrate reduction to ammonia (NO 3 − RR), as excessive *H often promotes the competing hydrogen evolution reaction (HER), leading to reduced Faradaic efficiency and ammonia yield. Herein, we address this issue by designing a single-atom Pd-doped Cu/Cu 2 O electrocatalyst (SA Pd–Cu/Cu 2 O) that precisely modulates *H generation and consumption. The SA Pd–Cu/Cu 2 O catalyst achieves an exceptional NH 3 yield rate of 1634.14 μg h −1 mg −1 , a NO 3 − –N conversion of 97.56%, a NH 3 –N selectivity of 98.13%, and a Faradaic efficiency of 92.13% at −0.8 V vs. RHE. In situ spectroscopic studies and density functional theory (DFT) calculations reveal that single-atom Pd sites serve as hydrogenation centers that generate moderate *H, which is efficiently consumed by nitrogen-containing intermediates, thereby suppressing HER. In contrast, nanoparticle Pd doping produces excess *H, favoring HER. This work demonstrates an innovative strategy for balancing *H utilization via atomic-scale metal doping, offering new insights into the design of high-selectivity electrocatalysts for sustainable ammonia synthesis and environmental nitrate remediation.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2026
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IF 2.6
Qian Wang,Rubo Fang,Heng Yuan,Xinyi Zhang,Guilong Hu,Qunfeng Zhang
To address the high consumption and cost of noble metal catalysts during the production of hexanitrohexaazaisowurtzitane (HNIW, CL-20), nitrogen-doped titanium dioxide (TN) was synthesized using urea as a nitrogen source. PdO/TN catalysts were then fabricated via a deposition–precipitation route and applied to the continuous hydrogenolysis debenzylation of hexabenzylhexaazaisowurtzitane (HBIW). Characterization by XRD, TEM, Raman, XPS, and H₂-TPR revealed that nitrogen incorporation effectively promoted the generation of surface oxygen vacancies and strengthened metal–support interactions, thereby enhancing catalyst stability. Moreover, the oxygen vacancy concentration could be tuned by adjusting calcination conditions. The PdO/TN-400-2 catalyst, prepared at 400 °C for 2 h, exhibited the highest catalytic activity, with an oxygen vacancy fraction of 19.64%. Further decreasing the calcination severity increased defect density but did not yield additional performance gains. These findings demonstrate that nitrogen doping can regulate surface defect chemistry and metal–support coupling, offering a viable strategy for the design of efficient catalysts for hexabenzylhexaazaisowurtzitane (HBIW) debenzylation.
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ACS Catalysis
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2026
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IF 13.6
Tianyao He,Yuzhen Zhang,Gan Li,Xiang Tu,Fengqing Zhuo,Jian Ji,Fengbo Yu,Guobo Li,Wenming Liu,Lu Wei,Jiguang Deng,Weili Dai,Honggen Peng
We report the rational design and precise construction of Y zeolite-encapsulated Pd catalysts featuring coexisting single atoms and clusters (Pd1+n@Y) that enable the efficient and low-temperature total oxidation of propane. Fine tuning of Pd loading and synthesis conditions in a PVP-assisted one-pot hydrothermal approach affords controllable confinement of dual active sites (isolated Pd single atoms and clusters). Catalytic evaluations reveal that Pd1+n@Y exhibits a T90 of only 265 °C, significantly outperforming the single-site counterparts (Pd1@Y and Pdn@Y). Combining density functional theory (DFT) calculations with in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies elucidates a stepwise synergistic mechanism wherein Pd single atoms preferentially activate the C–H bond in propane to form alkyl intermediates, while Pd clusters facilitate O2 activation and C–C bond cleavage to complete oxidation. This work establishes a robust “single atom–cluster” synergistic paradigm for designing advanced catalysts for the abatement of light alkanes.
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高影响因子
Journal of Environmental Sciences
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2026
·
IF 6.5
Weiwei Yang,Tengbin He,Weijie Huang,Yan Zhang,Wenpo Shan,Taicheng An
The geometric interplay in heterogeneous catalysis plays a crucial role in determining the catalytic performance. Based on the stronger affinity of Pd for ceria (CeO 2 ) than for titanium oxide (TiO 2 ) found in this work, we strategically engineered distinct Pd local environments by controlling the architecture of CeO x on TiO 2 through adjusting Ce content. At low Ce content, Pd preferentially assembles onto CeO x islands that are interspersed on TiO 2 ; while at high Ce content, Pd predominantly anchors onto the extensive CeO x surface. The former structure, enriched with CeO x -TiO 2 interface, exhibits superior capability in C-H bond cleavage and O 2 activation, leading to outstanding performance in the oxidation of carbon-containing gases such as light volatile organic compounds (VOCs; e.g., ethane and ethylene) and carbon monoxide (CO). In contrast, the structure dominated by continuous CeO 2 networks shows markedly lower activity. Combined analyses indicate that Pd 2+ species act as the primary active sites, and the consistent activity trend across differently Ce-modified catalysts in VOCs and CO oxidation can be explained by shared mechanistic steps, particularly through common CO and bicarbonate species intermediates. This work provides fundamental insight into the relationship between interfacial geometry and catalytic function.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2026
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IF 3.9
Xing Yan,Dongren Cai,Jiachang Li,Chuanlong Ran,Kok Bing Tan,Ahmad Zuhairi Abdullah,Sajid Ali,Yingfeng Chen,Guowu Zhan
Abstract Although Pd/ZrO2 represents a highly promising catalyst for CO2 hydrogenation, it still faces challenges such as low methanol selectivity and intense competing side reactions. In this study, we precisely constructed an In2O3 interfacial layer between Pd and ZrO2 by atomic layer deposition (denoted as Pd/xIn2O3/ZrO2, where x represents the number of atomic layer deposition cycles) and systematically investigated the role of this interlayer in modulating the catalyst microstructure, reaction pathways, and methanol selectivity. Catalytic performance evaluation results reveal that under reaction conditions of 320 °C and 3 MPa, the Pd/10In2O3/ZrO2 catalyst exhibits the best performance for CO2 hydrogenation to methanol, whereby the methanol selectivity was significantly enhanced from 6.6% to 76.6%, and the methanol space-time yield increased by approximately 6 times (2.40 vs. 13.37 gMeOH·gPd–1·h–1) when compared to pristine Pd/ZrO2 catalyst. Multifaceted characterization and in situ diffuse reflectance infrared Fourier transform spectroscopy demonstrate that the introduction of In2O3 substantially strengthens CO2 adsorption and activation, promotes further hydrogenation of the key CO* intermediate, and establishes a dual-path synergistic mechanism involving both formate and CO-hydrogenation routes, thereby effectively suppressing the formation of the byproduct CO. Collectively, this work demonstrates that catalyst interface engineering via atomic layer deposition provides an effective strategy for tuning the reaction network and optimizing methanol selectivity in catalytic CO2 hydrogenation systems.
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