ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.3
Ying Liang,Xianping Liao,Yingshuai Jia,Shiming Guan,Wanling Zhang,Wenbiao Zhang,Yuying Meng,Yi Tang,Qingsheng Gao
Electrooxidation offers a sustainable alternative by utilizing renewable energy to convert biomass-derived cyclohexanol (CHA) to adipic acid (AA), a key industrial chemical for nylon-66 and polyurethane production. While bimetallic Ni-based catalysts enhance the conversion, the role of secondary metals in modulating Ni active-site reconstruction during operation remains unclear, limiting performance optimization. Here, we demonstrate that Cr-doping promoted the dynamic reconstruction of Ni(OH)2 nanosheets to form NiOOH with abundant Ni3+ and oxygen vacancies (OVs), significantly boosting AA electrosynthesis. In situ characterizations reveal that Cr-doping accelerates OH– adsorption and promotes NiOOH formation, while subsequent Cr3+ leaching generates OVs, thus, resolving the long-standing dilemma between stabilizing high-valence Ni and maintaining abundant defects. The optimized catalyst achieves 78.1% AA yield and 85.4% Faradaic efficiency at 1.45 V vs RHE, outperforming undoped Ni(OH)2 and prior systems. Mechanistic studies identify surface Ni3+ and OVs-stabilized *OOH species as the keys for CHA dehydrogenation and cyclohexanone oxidation, respectively. Moreover, a membrane electrode assembly electrolyzer was designed for the efficient coproduction of AA (0.078 mmol h–1 cm–2) and H2 (42.9 mL h–1 cm–2) at a current density of 100 mA cm–2, demonstrating the scalability. This work clarifies the in situ reconstruction of bimetallic sites and provides a design strategy for the efficient electrosynthesis.
✓ 已验证
DOI
高影响因子
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
·
2026
·Vol. 131
·期 18
·e2026JD047458
·
IF 3.8
Ruidong Zhang,Kun Li,Yifan Zhou,Li Xu,Aijing Song,Jie Hu,Xiaowen Chen,Kuanyun Hu,Xueqi Ma,Huiwen Ding,Jianlong Li,Lin Du
Biomass burning (BB) emits large amounts of polycyclic aromatic hydrocarbons (PAHs) and is an important source of secondary organic aerosol (SOA). Recent studies suggest that, compared with gas-phase oxidation, the oxidation of BB-emitted organics in atmospheric aqueous phases can substantially enhance the formation of aqueous SOA (aqSOA). However, the aqueous-phase transformation and environmental fate of PAHs from BB remain poorly understood. This study reports the OH-initiated aqueous-phase oxidation kinetics and reaction mechanisms of three representative biomass-burning PAHs: naphthalene (NAP), acenaphthene (ACE), and acenaphthylene (ACY). The second-order aqueous-phase rate constants for reactions with OH were measured to be (1.63 ± 0.55) × 10 10 , (3.37 ± 1.15) × 10 10 , and (2.07 ± 0.70) × 10 10 M −1 s −1 for NAP, ACE, and ACY, respectively. The estimated aqueous-phase lifetimes were generally shorter than the corresponding gas-phase lifetimes under the representative OH conditions considered here, highlighting the potential importance of atmospheric aqueous environments in promoting the aging and transformation of these PAHs. Product analysis and pathway inference showed that NAP and ACE preferentially formed lower-carbon, more highly oxidized products, whereas ACY more readily produced oxygenated products that retained larger carbon skeletons. Furthermore, this study identified six previously unreported aqueous-phase oxidation products, reflecting ongoing oxidation and structure-dependent patterns of product evolution. Field observations showed that five newly identified products were also detected in ambient PM 2.5 samples, supporting the atmospheric relevance of the laboratory-identified products. These results improve our understanding of the aqueous-phase transformation of PAHs and their potential contribution to aqSOA formation.
✓ 已验证
DOI
高影响因子
Materials Today Chemistry
·
2026
·
IF 7.4
Dahong Peng,Hongkang Su,Ziting Yan,Chenxu Li,Shilie Pan,Min Zhang
A systematic comparison of F − /OH − modified [B 3 O 6 ] 3- clusters shows that properties evolve with F − /OH − content. • By changing the type and arrangement of the fundamental building blocks, a breakthrough in dimensionality was achieved. • Tunable optical properties were achieved, namely, the birefringence across the series ranges from 0.013 to 0.112 at 546 nm. Borates stand out as a prominent class of compounds in structural chemistry, acclaimed for their extraordinary structural diversity stemming from the versatile B–O fundamental building blocks (FBBs), and terminal oxygen modification has emerged as a powerful and effective strategy for tailoring their structures and optimizing functional properties. Herein, we report the synthesis of seven novel hydroxyfluorooxoborates with different dimensional framework via F − /OH − terminal modification of the isolated [B 3 O 6 ] 3- cluster, aiming to explore structural diversity and structure-property relationships. These compounds are classified by their FBBs: Compounds I-IV (A 7 [B 3 O 3 F 4 OH] 2 (PF 6 ) 3 , A = Rb, K, Cs, NH 4 ) with [B 3 O 3 F 4 (OH)] 2- ; Compounds V-VI (Cs 1.2 (NH 4 ) 0.8 [B 3 O 3 F 2 (OH) 2 ] 2 and Rb 1.7 K 0.3 [B 3 O 3 F 2 (OH) 2 ] 2 ) with [B 3 O 3 F 2 (OH) 2 ] - ; and Compound VII (Rb 7 [B 3 O 3 F 2 (OH) 2 ] 2 [B 3 O 3 F 4 (OH)](NO 3 ) 2 BF 4 ) with coexisting [B 3 O 3 F 4 (OH)] 2- and [B 3 O 3 F 2 (OH) 2 ] - . The birefringence across the series ranges from small (∼0.013 - 0.024 at 546 nm for I-IV) and moderate (∼0.051 at 546 nm for VII) to large (∼0.063 - 0.112 at 546 nm for V and VI). Structural and properties analyses reveal that F − /OH − substitution eliminates B–O dangling bonds of [B 3 O 6 ] 3- , leading to varied [B 3 O 3 F 2x (OH) 3−x ] (x = 1, 2, 3) and [B 3 O 3 (OH) x ] (x = 3, 4, 5, 6), featuring a distinct structure-property relationship. In the [B 3 O 3 (OH) x ] series, both polarizability anisotropy and band gap decrease with rising hydroxyl content, while hyperpolarizability increases. In contrast, the mixed F − /OH − series exhibit the opposite trend. In conclusion, this work significantly provides a rational synthetic strategy for tailoring FBBs and constructs deep-ultraviolet hydroxyfluorooxoborates with tunable optical performance. Through F − /OH − terminal modification of [B 3 O 6 ] clusters, a structural breakthrough from 0D clusters to a 2D layer was achieved, along with tunable optical properties. Download: Download high-res image (251KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
Waste and Biomass Valorization
·
2026
·
IF 3.1
Zhao Kunzhen,Zhang Zhuoma,Hang Xina,Yi LinLin,Li Kaiyuan,Zou Yanyan
Polyether ether ketone (PEEK) is a high-performance thermoplastic with considerable potential for H 2 and syngas productions via pyrolysis. However, its conventional non-catalytic pyrolysis suffers from high energy consumption and low H 2 and syngas yields. This study investigates the catalytic pyrolysis of PEEK using nickel hydroxide (Ni(OH) 2 ) to enhance the gas production efficiency. PEEK mixed with Ni(OH) 2 at different molar ratios (1:0–1:2) was pyrolyzed up to 1073 K under a nitrogen atmosphere. The H 2 yield increased with catalyst loading and reached a maximum of 25.9 mg/g at a PEEK: Ni(OH) 2 ratio of 1:0.5 (13.85 wt%), corresponding to a 264.3% increase compared with non-catalytic pyrolysis. The syngas yield also reached a maximum of 0.75 g/g under the same condition. Thermogravimetric analysis showed that the addition of Ni(OH) 2 significantly lowered the onset decomposition temperature of PEEK from 832 K to 532 K, and transformed its two-stage pyrolysis into a four-stage process with a 10.4% reduction in char residue. In-situ X-ray diffraction revealed that Ni(OH) 2 was progressively transformed into NiO and Ni during heating, indicating the formation of catalytically relevant Ni-containing phases within the pyrolysis temperature range. Scanning electron microscopy showed that the catalyst was distributed within the carbon matrix and altered the morphology of the pyrolysis residue. These observations provide qualitative evidence of morphological changes after catalytic pyrolysis. These findings demonstrate that the catalytic potential of Ni(OH) 2 in facilitating H 2 -rich syngas production from PEEK.
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Rongjing Jia,Shuling Chang,Ruirui Wang,Yanhong Xu,Rijie Wang,Lihong Zhang
The electrocatalytic CO 2 reduction reaction to CO (ECO 2 RR) is an effective way to achieve carbon resource utilization. It requires catalysts that can synergistically couple CO 2 activation with efficient CO desorption. This work engineers this synergy by constructing an interfacial Ag δ+ -O-Zn configuration on Zn(OH)F-derived supports via controlled Ag loading (0–5 wt%). The optimal catalyst (3A/Z, 3 wt% Ag) balances the formation of interfacial, oxidized Ag species (Ag δ+ ) with well-dispersed metallic Ag 0 nanoparticles. It achieves a CO Faradaic efficiency of 95.4% at −1.15 V vs. RHE and maintains 86% efficiency over 5 h at 6.38 mA cm −2 . In-situ ATR-SEIRAS spectra and kinetics reveal that Ag δ+ -related sites lower the barrier for *COOH formation, while adjacent Ag 0 domains facilitate *CO desorption. Excessive loading (5A/Z) promotes Ag aggregation and support decomposition, diminishing the critical Ag δ+ -O-Zn interface and performance. This study highlights interface coordination engineering as a key strategy for designing bifunctional ECO 2 RR catalysts.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Longyu Qiu,Menggang Li,Fenyang Tian,Lin He,Wenxin Zhu,Fengyu Wu,Xue Ren,Tongbo Zhang,Zhekai Zhang,Shipeng Zhang,Jiecai Han,Weiwei Yang,Yongsheng Yu
Proposing an in-plane N-bridged structure for atomic-level robust coordination. • Strong orbital overlap redirects hydroxy adsorption from Ni/Fe sites to Ru atoms. • Optimized coordination alleviates scaling relations and suppresses Ni site oxidation. • AEMWE achieves 2 A cm 2 at 1.84 V with ultra-stable operation over 800 h. The pursuit of high-performance anion exchange membrane water electrolysis (AEMWE) catalysts is limited by conventional supported and lattice-doped materials, which suffer from weak interfacial coupling and suboptimal intermediate adsorption, leading to degradation under industrial conditions. Although atomic-level modulation is highly appealing, achieving a synergistic balance between robust structural stability and precise control over the reaction pathway remains challenging. Herein, by employing a nitrogen-coordinated metal bridging strategy, we report a Ru-NiFeN with atomically coordinated Ru-N bridges for practical water electrolysis. This configuration manipulates the local electronic microenvironment to trigger a site-specific redirection of OH adsorption from Fe to Ru centers, effectively bypassing host-lattice scaling-relation limitations and lowering OER barriers. In-situ spectroscopy and theoretical calculations reveal that the Ru-N bridge promotes resilient dynamic structural reconstruction, enabling potential-triggered NiOOH formation while suppressing detrimental metal oxidation. The Ru-NiFeN catalyst achieves a low overpotential of 340 mV at 1 A cm 2 and demonstrates outstanding AEMWE durability, operating for over 800 h at 2 A cm 2 with a decay rate of only 24.4 μV h 1 , positioning it among the most active catalysts reported. This work provides a strategic pathway for optimizing adsorption landscapes via atomic coordination engineering for efficient, stable energy conversion. Download: Download high-res image (191KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2026
·
IF 4
Tao Liu,Donglong Fu,Cuncun Wu,Xianhua Zhang,Gamal Sewify,Mohamed Mokhtar Mostafa,Sai Chen,Chunlei Pei,Zhi-Jian Zhao,Jinlong Gong
Hydroxy groups derived from water dissociation play a crucial role in reforming chemistry. A direct experimental verification of interfacial hydroxy groups, however, together with the precise control of active -OH species for hydrogen production has not been obtained. This paper describes an interface engineering strategy to modulate active -OH species for hydrogen production from methanol steam reforming. Based on comprehensive in-situ spectroscopic characterizations, the normalized bridged Ce3+-OH species present linear correlation with the copper-ceria interface density, suggesting that bridged Ce3+-OH species are mainly adsorbed at the copper-ceria interface. The bridged Ce3+-OH species adsorbed at interfacial sites are demonstrated as the primary active configurations that react with methoxy groups to generate formate species, thereby enhancing hydrogen production in low-temperature methanol steam reforming, achieving an optimal TOFH2 of approximately 956 h-1 at 220℃. This work provides a profound insight into the intrinsic reaction at the metal-support interfacial sites for the reforming chemistry.
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2026
·
IF 29.1
Zhihao Sun,Lin Liu,Junwei Zhang,Yuhang Liu,Yifeng Wang,Ying Wan,Fanxing Bu,Bao Zhang,Wanhai Zhou,Dongyuan Zhao,Dongliang Chao
Unlike neutral aqueous batteries with cationic Zn 2+ as the charge carrier, alkaline batteries with anionic [Zn(OH) 4 ] 2‒ and OH ‒ are actually commercially feasible and thermodynamically stable thanks to their ability to suppress hydrogen evolution. Whereas commercial separators in alkaline batteries, without ion regulation capability, fail to suppress severe dendrite and passivation of anionic [Zn(OH) 4 ] 2‒ and accelerate ion transport of anionic OH ‒ . Herein, we tailor the coordination structures of alkali-stable cationic complexes in polymer separators (CCPS) to construct anionic OH ‒ selective transfer channels. Synchrotron spectroscopic characterizations and theoretical calculations reveal that the low-coordination cationic complexes expose more positive charge density, electrostatically attracting more negative charge from [Zn(OH) 4 ] 2‒ . In situ electrochemical digital holography technology and time-of-flight secondary ion mass spectrometry analyses further confirm the homogeneous [Zn(OH) 4 ] 2‒ distribution at the CCPS-electrode interface, oriented Zn deposition, and impeded passivation. As a result, CCPS enables alkaline Zn||Cu cells to operate over 5500 cycles at 1 mA cm ‒2 with a high coulombic efficiency of 99.99%. Alkaline Ni–Zn batteries exhibit ultrastable cycling over 1000 cycles at 6 C and maintain 86.17% of their maximum capacity at 10 C. Our work may provide practical and effective separator strategies to accelerate the commercialization of alkaline batteries.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Song He,Junqing Zhu,Jiayi Tang,Jinfeng Ji,Yajun Huang,Ye Li
Metal-organic frameworks (MOFs) have become a focal point of interest owing to their ability to remove contaminants from wastewater. However, the typical powder form of MOFs is difficult to recover after use, which hinders their practical application. In this research, UiO-66-OH gel was synthesized at room temperature. On this basis, Co was doped into UiO-66-OH gel to obtain a series of Co@U-OH-X composites. The [email protected] exhibited an adsorption capacity for TC that was 5.1 times higher compared to the UiO-66-OH gel. Furthermore, the influence of pH, coexisting ions, humic acid, and original concentration of TC on the adsorption of [email protected] was examined. The composite materials demonstrated an exceptional capacity to adsorb TC (182.31 mg·g -1 ), which surpassed the performance of numerous previously documented adsorbents. The pseudo-second-order kinetic model and the Freundlich isotherm model efficiently accounted for the adsorptive interaction. Thermodynamic adsorption analyses indicated that the interaction occurred spontaneously and accompanied by heat absorption. After four cycles, there was only a 12.7% reduction in the removal rate of TC, which suggested that the composite materials were recyclable. [email protected] showed remarkable adsorption capacity even in settings with minimal TC concentration. The exceptional adsorptive performance, superior recyclability and aqueous stability established Co@U-OH-X composites as a viable adsorbent contender for eliminating TC.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Shencheng Pan,Min Bi,Jingyi Wang,Zhouping Jiang,Yan Zhou,Zhen Wu,Xin Wang,Junwu Zhu,Yongsheng Fu
Surface-oxidized RuCu single-atom alloy synthesized via PLIL. • Ultrafine ~3 nm particles with atomically dispersed Cu and surface oxide. • Downshifted d-band center weakens *OH adsorption and optimizes ΔG H . • Superior alkaline HER: 27.5 mV@10 mA cm −2 , Tafel 24.2 mV dec −1 . • Synergistic Cu and surface oxidation modulation enhances water dissociation. Hydrogen evolution reaction (HER) in alkaline media is severely hindered by sluggish water dissociation kinetics and the strong adsorption of hydroxyl intermediates (*OH). Herein, we report a surface-oxidized RuCu single-atom alloy (RuCuO) supported on carbon nanotubes, synthesized via a pulsed laser irradiation in liquids (PLIL) strategy. The resulting catalyst features ultrafine nanoparticles (~3 nm) with atomically dispersed Cu and an in situ formed surface oxide layer. Benefiting from the synergistic electronic modulation induced by Cu incorporation and surface oxidation, the d-band center of Ru is downshifted, leading to weakened *OH adsorption and optimized hydrogen adsorption free energy (ΔG H ). As a result, RuCuO exhibits outstanding HER performance in alkaline media, delivering a low overpotential of 27.5 mV at 10 mA cm −2 and a small Tafel slope of 24.2 mV dec −1 , surpassing commercial Pt/C. Mechanistic investigations combining X-ray absorption spectroscopy and density functional theory calculations reveal that the surface oxide layer not only suppresses *OH poisoning but also enhances H 2 O adsorption and dissociation. This work provides a viable strategy for designing high-performance alkaline HER catalysts through surface oxidation engineering of single-atom alloys. A surface-oxidized RuCu nanoalloy was prepared via pulsed laser irradiation in liquids (PLIL), enabling in situ surface oxidation and electronic structure modulation. The optimized surface electronic environment tunes OH adsorption and delivers enhanced hydrogen evolution activity. Download: Download high-res image (126KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
Environmental Science-Nano
·
2023
·Vol. 10
·期 4
·1109-1125
·
IF 7.3
Xiao Huang,Wen Yan,Jingxiang Sun,Tao Hu,Jinxi Feng,Zhen Huang,Shuanghong Tian,Ya Xiong
The achievement of highly active and stable piezocatalysts is still challenging for the efficient transformation of mechanical energy to chemical energy. Herein various SnOxHy species were prepared by a simple precipitation–thermal treatment method and applied for the piezocatalytic degradation of tricyclazole. It is found that the catalytic activity depended on the thermal treatment and follows the order SnO(OH)2 (80 °C) > SnO2.55H1.1 (200 °C) > SnO2.3H0.6 (300 °C) > SnO2.22H0.24 (400 °C) > SnO2 (500 °C) > rutile SnO2 (800 °C). SnO(OH)2 (80 °C) boosted the degradation of tricyclazole and the reaction constant reached as high as 0.0354 min−1, 7.1 fold that of SnO2 (800 °C). The differences among these SnOxOHy piezocatalysts mainly stemmed from the dissimilarity of the relative content of SnO(OH)2. In addition to the Sn–O piezoelectric motif, SnO(OH)2 had rich hydrogen bond networks, which work like molecular springs under external pressure. Due to such a special structure, SnO(OH)2 had not only a super high piezoelectric constant (d33) of 409.1 pm V−1 among the currently reported piezomaterials, but also a 0.49 eV-higher valence band than SnO2, being beneficial to the generation of stronger oxidative ˙OH. This is the first example of inorganic hydrogen-bonded piezomaterials, which opens a new window to develop advanced piezocatalysts for highly efficient degradation of refractory pollutants by piezocatalysis.
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2023
·
IF 17.1
Chuansheng He,Linlin Yang,Xiaohui Peng,Shangheng Liu,Jia Wang,Chengyuan Dong,Delin Du,Leigang Li,Lingzheng Bu,Xiaoqing Huang
Thickness regulation of transition metal hydroxides/oxides nanosheets with superior catalytic properties represents a promising strategy to enhance catalytic performance, but it remains an enormous challenge to achieve precise control, especially when it comes to the ultrathin limit (several atomic layers). In this work, a facile strategy of alkylamine-confined growth is proposed for the synthesis of thickness-tunable metal hydroxide/oxide nanosheets. Specifically, ultrathin cobalt hydroxide and cobaltous oxide hybrid (Co(OH)2-CoO) nanosheets (Co–O NSs) with a thickness in the range of 2–6 nm (5–13 atomic layers) are synthesized by using alkylamines with different carbon chain lengths as the ligand to modulate vertical coordination ability. Co–O NSs with a thickness of 2 nm (Co–O NSs-2 nm) exhibit excellent oxygen evolution reaction (OER) performance with an overpotential of 278 mV at 10 mA/cm2. The maximized number of active sites including oxygen vacancies, optimal adsorption strength, and the highest electrical conductivity are considered as the potential factors contributing to the excellent OER performance of Co–O NSs-2 nm. This work holds great significance for the precise thickness-tunable synthesis of transition metal layered hydroxide nanosheets with modulated and improved catalytic performance.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）