Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124167
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IF 7.5
Chen Chen,Zhenyu Wang,Yasen Li,Jiayao Gao,Xin Chen,Mingjie Jia,Die Shao,Yiming Wang,Xuejian Li,Fuqiang Yu,Guangwen Xu,Junli Xu,Hong-bin Sun
Transition-metal borides have long been developed as promising electrocatalysts for the hydrogen evolution reaction (HER); however, the identity of their true active phase remains controversial. Here, in conjunction with our previous studies, by systematically investigating a series of cobalt- and nickel-boride-derived catalysts through a combined computational and experimental screening, we reveal that HER activity universally originates from the synergistic interaction between metallic sites and hydroxide matrices, enabled by lattice expansion, interfacial electronic transfer, and dynamic surface evolution. As a representative high-performance example, Pt-modified Co(OH) 2 derived from cobalt boride exhibits ultralow overpotentials of 11 mV at 10 mA cm −2 and 95 mV at 500 mA cm −2 , together with long-term stability. Importantly, the same reconstruction principle applies to Ni-boride systems, confirming the generality of this approach. Beyond water electrolysis, we further demonstrate that these HER catalysts are highly effective in Al-H 2 O batteries, where hydrogen evolution is coupled with electrical energy harvest. An alkaline Al-H 2 O battery employing the reconstructed catalyst delivers a power density of 21.96 mW cm −2 . This work establishes that the activity of “boride-based” HER catalysts fundamentally arises from reconstructed metal-hydroxide active centers, providing a development paradigm of transition-metal electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Guocui Cai,Helong Jiang,Fangyi Chu,Xiangcun Li,Xiaobin Jiang,Xiao Wu,Gaohong He,Yan Dai
Here, the conventionally disordered Co(OH)F filaments are rearranged to form highly-ordered flower-like Co(OH)F architectures in a conductive membrane substrate. The important findings contribute to designing delicate nanostructures and improving the catalytic activity of advanced materials for energy applications. The hierarchically porous CNT@NC membrane with CNT as the core and N -doped carbon as the crosslinking shell is scalably designed firstly for strengthening the transport of Li + and electrons in the electrode, providing an ultrahigh porosity for growing flower-like Co(OH)F on both surfaces and interior of the membrane, as well as offering electrons for the redox reactions through the roots of the Co(OH)F flowers. Furthermore, the ordered Co(OH)F bundles with divergent and open-ended structures provide the catalyst with the broad reaction interface and active sites for polysulfides (LiPSs) anchoring and catalytic conversion at a low energy barrier, significantly facilitating the diffusion of ions and electrolyte in the catalyst, and thus effectively alleviating the shuttle effect. Owing to the synergistic effect between the conductive membrane substrate and the grown Co(OH)F catalyst, the Co(OH)F-CNT@NC cathode generates a high reversible capacity and excellent long-term cycling performance (622 mAh·g −1 at 1C after 600 cycles). Conclusively, the proposed facile strategy provides insights regarding the design of novel cathode materials for high-areal-capacity Li–S batteries.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Yulan Song,Cuilan Tang,Tao Wang,Yansong Liu,Xiaoshan He,Chunping Xie,Guo Chen,Chengfu Deng,Zhibing He,Jinglin Huang
Constructing electronic structures with abundant surface/interface structures and effective regulation of catalytic active centers is an effective strategy to improve electrocatalytic performance, but designing efficient bifunctional non-noble metal oxygen evolution reaction (OER) and urea oxidation reaction (UOR) electrocatalysts remains challenging. Studies have shown that p-n heterojunctions can effectively regulate the electronic structure of catalytic active sites while having abundant surface/interface structure, which plays an important role in improving the native catalytic activity. Herein, FeNi-OH/Co(OH) 2 /NF p-n heterojunction structure was constructed by a simple electrochemical deposition method, and the effects of content, deposition time, and number of cycles on catalytic performance were investigated. The results show that Fe(0.02 M)Ni(0.07 M)–OH(100 s)/Co(OH) 2 (5)/NF composite material has the best OER and UOR catalytic performance. For OER, the electrocatalyst only requires an overpotential of 271 mV to obtain a current density of 50 mA cm −2 , and an applied voltage of 1.56 V to obtain a total water decomposition of 10 mA cm −2 (FeNi-OH/Co(OH) 2 /NF||Pt). For UOR, a voltage of only 1.314 V ( vs. RHE) is required to achieve a current density of 10 mA cm −2 , and an applied voltage of 1.44 V can achieve a current density of 10 mA cm −2 . Experimental, in situ measurements and theoretical results indicate that the improvement in catalytic activity is mainly due to the potential difference between FeNi-OH and Co(OH) 2 , which induces self-driven charge transfer at the interface, promoting the adsorption of reactant molecules, optimizing reaction barriers, accelerating chemical bond cleavage, and thus promoting catalytic reactions.
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Journal of Energy Storage
·
2026
·
IF 10.7
Yongbo Liu,Yang Chen,Limei Song,Jianhua Gao
In the field of electrochemical energy storage, polyanionic compounds exhibit outstanding electrochemical performance owing to their stable crystal structures and tunable operating potentials. Among these, vanadium-based phosphates stand out and have been extensively investigated. In this work, a novel polyanionic compound, Na 3 V(OH)(HPO 4 )(PO 4 ), was synthesized by a simple one-step hydrothermal method. Its crystal structure, confirmed by Rietveld refinement of the X-ray diffraction data, can accommodate sodium ions and provide open interstitial pathways to facilitate Na + diffusion, suggesting its potential as a cathode material for sodium-ion batteries (SIBs). Bond valence sum analysis and density functional theory calculations further validated the high Na + ion transport efficiency within the framework. Based on these findings, a half-cell was assembled using the as-prepared material as the cathode and metallic sodium as the anode. Electrochemical tests demonstrated excellent reversible cycling stability and rate capability, underscoring the promise of Na 3 V(OH)(HPO 4 )(PO 4 ) as a high-performance cathode candidate for SIBs.
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JOURNAL OF LUMINESCENCE
·
2025
·
IF 3.6
Yue Wang,Yaomin Lei,Wuqin Chen,Ruian Yang,Xinyang Gu,Gaofeng Pan,Xuesong Zhai,Jinshan Wang
Luminescence quenching effect of lanthanide-doped upconversion materials occurs with high probability even in larger-sized particles, but their main quenching pathway remains controversial. In this work, we investigate the influence of the surfactant and pH value on the luminescence properties of β-NaLuF 4 :Yb,Er microcrystals. A convincing evidence can be provided by the combination of X-ray diffraction (XRD), inductively coupled plasma (ICP) spectrometer, and Eu 3+ structural probe measurements that the major quenching pathway comes from the fast energy migration from the excited lanthanides to nearby OH − defects in the crystal lattice rather than surface quenching effect. Even at OH − -rich reactant condition, the upconversion luminescence intensity becomes more efficient by reduced internal quenching effects. Our findings provide a new and fundamental understanding of severe luminescence quenching effect at microscale, thus guiding the design and preparation of highly efficient upconversion materials.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Lu Zheng,Saisai Ju,Xiong Li,Yongde Ma,Hongwei Zhang,Zhenping Cai,Yanning Cao,Kuan Huang,Lilong Jiang
Efficient capture of residual NH₃ from Haber-Bosch recycling gas is essential to improve process efficiency and reduce environmental impact. In this study, a series of sulfonated porous organic polymers (PTO-1S, PTT-1S, PTF-1S) were fabricated by a post-sulfonation strategy using phenolic hydroxyl-containing precursors to capture NH 3 . Comprehensive characterizations of the sulfonated derivatives demonstrated not only the successful grafting of –SO₃H groups, but more importantly, a cooperative effect with the native phenolic –OH groups. The optimized PTO-1S achieves an outstanding NH₃ capacity of 11.52 mmol/g (at 298.2 K and 1 bar), with particularly impressive performance at low pressures (5.56 mmol/g at 313.2 K and 0.03 bar), surpassing most reported adsorbents. Mechanistic studies revealed that this cooperation creates an optimal balance of strong chemisorption (–SO₃H) and reversible hydrogen bonding (–OH), which is identified as the origin of the high capacity and exceptional cycling stability (< 1% capacity loss/cycle). Besides, the sulfonated samples maintain excellent selectivity under simulated industrial conditions (NH₃/N₂/H₂ mixtures) and a rapid adsorption rate (90% saturation within 2 min), demonstrating their potential for practical NH₃ recovery applications.
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Journal of Materials Chemistry C
·
2024
·Vol. 12
·期 34
·13632-13638
·
IF 5.7
Wenjing Tan,Xuefan Wang,Ruqing Wei,Hongbo Huang,Daqing Yang,Ying Wang,Bingbing Zhang
Nonlinear optical (NLO) crystals are crucial components in all-solid-state lasers because they expand the wavelengths of existing laser sources through laser frequency conversion. In this work, Ag2[TeO2(OH)4] was identified in tellurates using the first-principles high-throughput screening pipeline for NLO materials (FHSP-NLO). The material was successfully produced via mild aqueous solution synthesis conditions, and a single crystal of 8 × 4 × 4 mm3 in size was obtained. Ag2[TeO2(OH)4] is one of the few materials that contains the [TeO2(OH)4]2− anionic group and belongs to the non-centrosymmetric (NCS) space group. Ag2[TeO2(OH)4] exhibited balanced comprehensive performances, including a large second harmonic generation (SHG) response of about 0.84 × AgGaS2 (AGS), moderate band gap (2.73 eV) and large birefringence (0.106@1064 nm). First-principles studies revealed that the dominant units that contribute to the crystal's linear and nonlinear optical properties are Ag atoms and TeO2(OH)4 groups.
研究领域:
材料科学
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光学
·
无机化学
·
计算物理
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Yuyu Li,Fang Luo,Yuhua Xie,Chaofeng Chang,Ming Xie,Zehui Yang
Urea oxidation reaction (UOR) is a promising substitution of oxygen evolution reaction (OER) in overall water splitting technology because of the lower theoretical potential; thereby, a win-win benefit is achieved due to the simultaneous hydrogen generation and water purification . The efficient UOR catalysis substantially depends on the exposed active sites and mass transfer resistance, especially at high current density to meet the requirement of industrial water splitting technology. In this work, we have synthesized α-Ni(OH) 2 porous nanoflowers (α-Ni(OH) 2 –PNF) using ZIF-67 as template. Ascribing to the Kirkendall effect , nanopores are created on α-Ni(OH) 2 nanosheets benefiting for the formation of abundant oxygen vacancies as well as drop-off in mass transfer resistance during UOR catalysis. Meanwhile, the binding strength between active site and CO 2 , rate-determining step of UOR, is weakened by oxygen vacancies; as a result, only 1.477 V vs. RHE is demanded for α-Ni(OH) 2 –PNF to catalyze UOR with 100 mA cm −2 , 67 mV lower than α-Ni(OH) 2 nanosheets. Besides, an exceptional stability is also achieved for α-Ni(OH) 2 –PNF with negligible degradation during 20 h catalysis.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 48
·期 8
·3347-3357
·
IF 3.134
Zhang Xiangxiang,Zhou Man,Zhong Yang,Zhang Letian,Kang Jianjian,Wang Lingzhi
Co(OH) 2 modified TiO 2 (Co(OH) 2 /TiO 2 ) was fabricated by a simple precipitation method and applied as a surface enhanced Raman scattering (SERS) substrate. Using triphenylmethane dye acid blue 83 as the analyte, the SERS substrate showed high sensitivity with a detection limit of 1 × 10 –7 M and high signal reproducibility with a relative standard deviation of 8.9%. Moreover, the substrate can also be used to in situ monitor the catalytic degradation of Acid blue 83. In addition, compared with cationic triphenylmethane dye, the Co(OH) 2 /TiO 2 substrate presented stronger SERS activity towards anionic counterparts. The easy preparation and high sensitivity and selectivity towards anionic dyes of Co(OH) 2 /TiO 2 provides a robust alternative for promoting the practical application of semiconductor-based SERS substrate in selective detection.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yanzhou Ding,Yiwen Zhu,Xia Yu,Shuguang Lyu,Yanlin Wu,Lei Zhou,Qian Sui
Antibiotic residues in aquatic environments can be effectively degraded by hydroxyl radical ( OH)-based advanced oxidation processes (AOPs). However, the reaction kinetics and mechanisms have not been comprehensive determined due to the limitations of conventional competition kinetic methods and mass spectrometry-based product identification, as these methods fail to exclude interference from secondary radicals and are unable to capture unstable intermediates or transient species. In this study, these limitations were overcome using laser flash photolysis (LFP) and density functional theory (DFT) calculations, allowing accurate determination of the OH-initiated reaction kinetics and degradation mechanisms of florfenicol (FF), a model veterinary antibiotic compound that is frequently detected in the environment. Based on the LFP experiment results, the second order rate constant ( k ) between OH and FF was determined to be 1.96 × 10 9 M −1 s −1 by tracking the typical signal of (SCN) 2 − . Furthermore, DFT calculations revealed two distinct mechanisms for OH addition to the benzene ring and identified hydrogen atom abstraction (HAA) reaction from chiral carbons as being the most favorable initial reaction for OH. In addition, the destruction of chlorine moiety occurred via hydroxylation-chlorine abstraction, rather than direct chlorine abstraction or substitution reactions. The resistance of chlorine moiety to degradation during the initial oxidation process, resulted in the formation of chlorine-containing by-products. This study provided a novel approach to comprehensively investigate the mechanisms of emerging contaminants elimination during OH-based AOPs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jia Deng,Xiang Zhan,Feng Wu,Shuxian Gao,Li-Zhi Huang
Trichloroethylene (TCE), one of the most frequently detected chlorinated organic pollutants (COPs) in groundwater, has potential risks to human health. The bimetallic system consisting of zero-valent iron (ZVI) and a second catalytic metal has been widely investigated for reductive dechlorination of COPs. However, the passivation layer of ZVI inhibits the electron transfer causing a low dechlorination efficiency. In this work, we designed a novel bimetallic system using Fe(OH) 2 and Ni for fast dechlorination of TCE. The reduction efficiency of TCE reaches 94.8 % after 5 h of reaction in the Fe(OH) 2 /Ni system. TCE was completely dechlorinated to nontoxic gas products including ethylene and ethane, which was attributed to the generation of active hydrogen species (H*) in the system. The Ni 2+ cations undergo the process of hydroxylation and olation. Subsequently, electrons of Fe(OH) 2 were transferred to Ni(II) causing the formation of Ni(0). The catalytic Ni(0) sites generate H* for TCE dechlorination via catalytic reduction of H 2 O/H + . A part of Fe(II) in the Fe hydroxide layer of Fe(OH) 2 was oxidized to Fe(III) leading to the formation of green rust with a hexagonal structure. Our work demonstrates Fe(OH) 2 /Ni is a promising composite material for the remediation of TCE-contaminated groundwater.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Wenjing Xie,Peng Zhang,Wenjuan Liao,Man Tong,Songhu Yuan
The potential of oxygenating Fe(II)-bearing sediments for hydroxyl radical (·OH) production and contaminant degradation has been proposed recently. Here, we further show that specific ligands can largely enhance contaminant degradation during sediment oxygenation due to increased utilization efficiency of sediment electrons. With the addition of 0–2 mM sodium ethylene diamine tetraacetate (EDTA) or sodium tripolyphosphate (TPP) in sediment suspension (50 g/L, pH 7.0), trichloroethylene (TCE, 15 μM) degradation increased from 13% without ligand to a maximum of 80% with 2 mM TPP and was much higher with TPP than EDTA because EDTA competes for ·OH. Electron utilization efficiency for ·OH production increased with increased ligand concentration and was enhanced by up to 6–7 times with 2 mM EDTA or TPP. Electron transfer from sediment to dissolved Fe(III)-ligand is mainly accountable for the enhanced electron utilization efficiency by the ligands with low adsorption affinity (i.e., EDTA), and additional variation of sediment surface Fe(II) coordination is mainly responsible for the enhancement by the ligands with high adsorption affinity (i.e., TPP). Output of this study provides guidance and optional strategies for enhancing contaminant degradation during sediment oxygenation.
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