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Water · 2017 ·Vol. 9 ·期 8 ·563 · IF 1.832

Study on Effects of Electron Donors on Phosphine Production from Anaerobic Activated Sludge

Jianping Cao,Chaosheng Zhang,Hongwei Rong,Meihua Zhao,Wei Wei,Limin Zhao

The effects of different types and concentrations of electron donors (glucose, starch, methanol and sodium acetate) on the formation of phosphine from anaerobic activated sludge that has been domesticated for a prolonged period were studied in small batch experiments. The results show that types and concentrations of electron donor have significant effects on the production of phosphine from anaerobic activated sludge. Among them, glucose was the most favourable electron donor, whereas sodium acetate was the least favourable electron donor for the removal of phosphorus and the production of phosphine. Higher concentrations of electron donors were more favourable for the reduction of phosphate into phosphine, and supplying more than nine times the amount of electron donor as theoretically required for the reduction of phosphate into phosphine was favourable for the production of phosphine.Keywords:anaerobic activated sludge;electron donor;phosphine;matrix-bound phosphine (MBP)

研究领域: 环境生物学 · 废水处理
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AICHE JOURNAL · 2021 ·Vol. 67 ·期 6 ·e17177 · IF 3.993

Integrating pore interconnectivity and adaptability in a single crystal hierarchical zeolite for liquid alkylation

Baoyu Liu,Jiajin Huang,Zhantu Liao,Chongzhi Zhu,Qiaoli Chen,Guan Sheng,Yihan Zhu,Yi Huang,Jinxiang Dong

Zeolite belongs to one of the most important families of solid acid catalysts in chemical industries. It is, however, severely constrained by the diffusion limitation for bulky molecules, a lack of multifunctionality for sequential reactions and pore adaptability toward specific adsorbates due to its small micropore size and simple aluminosilicate framework. Introducing mesopores into a zeolite toward realizing hierarchical zeolites is a prevailing strategy but one that usually suffers from compromised crystallinity as well as insufficient interconnectivity and openness of the mesopores. Herein, a novel acid-redox co-functionalized single-crystalline zeolite with highly open and interconnected mesopores is designed and fabricated. As a proof-of-concept study, we integrate solid acid and Fe-oxy redox sites into a hierarchical MEL zeolite with well-characterized microporosity and mesoporosity. This zeolite exhibits superior activity and stability toward alkylation between mesitylene with benzyl alcohol, arising from greatly facilitated intra-crystal molecular diffusion, mitigated metal leaching and optimized adsorbate-pore wall interactions.

研究领域: 化学工程 · 催化材料科学
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-12 · IF 16.6

Coupling acid catalysis and selective oxidation over MoO3-Fe2O3 for chemical looping oxidative dehydrogenation of propane

Wang Xianhui,Pei Chunlei,Zhao Zhi-Jian,Chen Sai,Li Xinyu,Sun Jiachen,Song Hongbo,Sun Guodong,Wang Wei,Chang Xin,Zhang Xianhua,Gong Jinlong

Redox catalysts play a vital role in chemical looping oxidative dehydrogenation processes, which have recently been considered to be a promising prospect for propylene production. This work describes the coupling of surface acid catalysis and selective oxidation from lattice oxygen over MoO 3 -Fe 2 O 3 redox catalysts for promoted propylene production. Atomically dispersed Mo species over γ-Fe 2 O 3 introduce effective acid sites for the promotion of propane conversion. In addition, Mo could also regulate the lattice oxygen activity, which makes the oxygen species from the reduction of γ-Fe 2 O 3 to Fe 3 O 4 contribute to selectively oxidative dehydrogenation instead of over-oxidation in pristine γ-Fe 2 O 3 . The enhanced surface acidity, coupled with proper lattice oxygen activity, leads to a higher surface reaction rate and moderate oxygen diffusion rate. Consequently, this coupling strategy achieves a robust performance with 49% of propane conversion and 90% of propylene selectivity for at least 300 redox cycles and ultimately demonstrates a potential design strategy for more advanced redox catalysts.

CAS / MDL: 7782-61-8
研究领域: 化学工程 · 催化科学
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2023 ·Vol. 98 ·期 9 ·2224-2234 · IF 3.4

Iron/carbon conductive materials for enhancing anaerobic treatment of synthetic acrylamide wastewater

Hao Fu,Yongwen Ma,Jinquan Wan,Yan Wang,Yingping Long,Jianye Cao

BACKGROUND Most studies have focused on the degradation of acrylamide (AM) by a single strain. There are relatively few studies on the treatment of AM by anaerobic activated sludge. Previous studies have shown that conductive particles can change the mode of electron transport between anaerobic microorganisms. Therefore, this study compared the enhancement effect of three different particles (Fe 3 O 4 , granular activated carbon (GAC), graphite) on the treatment of synthetic AM wastewater by anaerobic activated sludge under different temperature conditions (30, 25, 20 °C) and particle dose (2, 6 g L −1 ). RESULTS The results showed that 6 g L −1 GAC improved the removal rate of chemical oxygen demand (COD) and AM by 22.95% and 19% compared with the control group at 30 °C, respectively, indicating that the addition of GAC contributes to the degradation of AM and improves COD removal rate. Results of high-performance liquid chromatography (HPLC) showed that the activated sludge with GAC obviously promoted the degradation of AM. Besides, a large amount of propionic acid was detected in all experimental groups during the reaction, and the activated sludge with GAC promoted degradation of propionic acid. CONCLUSION Anaerobic activated sludge supplemented with sufficient GAC can not only absorb and degrade AM synchronously but also accelerate the conversion of intermediates, such as acrylic and propionic acids. Based on the results of HPLC and liquid chromatography–mass spectrometry, a possible method of degradation of AM by anaerobic activated sludge was proposed. © 2023 Society of Chemical Industry (SCI).

研究领域: 环境科学 · 微生物学
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ACS Catalysis · 2017 · IF 10.614

Enhanced Lattice Oxygen Reactivity over Ni-Modified WO3-Based Redox Catalysts for Chemical Looping Partial Oxidation of Methane

Sai Chen,Liang Zeng,Hao Tian,Xinyu Li,Jinlong Gong

Partially oxidizing methane into syngas via a two-step chemical looping scheme is a promising option for methane transformation. Providing the optimum lattice oxygen to selectively produce syngas represents the major challenge for the development of oxygen carrier materials in chemical looping processes. This paper describes the design of WO3-based oxygen carriers as the primary source of lattice oxygen with high melting points and attractive syngas selectivity. To further enhance the lattice oxygen availability and methane conversion capacity, NiO nanoclusters are introduced, considering the doping effect on chemical bonding disruption in both bulk and surface regions. For Ni0.5WOx/Al2O3, the nickel cations incorporated into the bulk of WO3 can strongly weaken the tungsten–oxygen bond strength and increase the availability of lattice oxygen. The surface-grafted nickel species can effectively activate methane molecules and catalyze the partial oxidation reaction. Total methane conversion and syngas yield can be substantially increased by about 2.7-fold in comparison with unmodified WO3/Al2O3. This work demonstrates that the bulk and surface modifications are feasible to tailor the active lattice oxygen of oxygen-carrying materials in chemical looping processes.

研究领域: 催化化学 · 能源化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Assembly of sphere-structured MnO2 for total oxidation of propane: Structure-activity relationship and reaction mechanism determination

Chao Feng,Gaoyan Xiong,Fei Jiang,Qianqian Gao,Chong Chen,Yuan Pan,Zhaoyang Fei,Yanpeng Li,Yukun Lu,Chenguang Liu,Yunqi Liu

Through morphology control and structure construction of manganese catalyst to improve the conversion of VOCs is still a significant challenge in the field of environmental catalysis. Herein, secondary sphere structured δ-type manganese oxide (MnO 2 -SS) was synthesized via a simple room temperature two-step method. Compared with other sphere-type MnO 2 samples, MnO 2 -SS exhibited a higher propane oxidation activity (T 90  = 238 ℃), turnover frequency (14.54 × 10 −7 s −1 at 240 ℃), and stability in H 2 O, NO 2 , and CO atmospheres. Experimental results indicated that MnO 2 -SS exhibited an ultrahigh specific surface area, a high surface concentration of active Mn 4+ species and superior surface oxygen mobility. In-situ DRIFTs revealed that active oxygen species exhibit a key role in formation and dissociation of intermediate carboxylates. Electron paramagnetic resonance, O K-edge results and density functional theory calculation revealed that numerous oxygen vacancies existed on MnO 2 -SS. These vacancies can facilitate adsorption and activation of O 2 to generate active reactive oxygen species, which lead to superior propane and intermediate carboxylates oxidation activity. This work provides new strategy to enhance the surface oxygen activity of manganese oxide.

研究领域: 环境催化 · 材料科学 · 化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Heteroatom/Flexibility-Adaptive carbon electrode via Shallow-Etching strategy enables Long-Life Zinc-Air batteries

Wenhua Shi,Xiangjun Zheng,Jiahui Wang,Xiujie Wang,Xingmei Guo,Yuanjun Liu,Junhao Zhang,Xuecheng Cao,Ruizhi Yang

Integrating catalytic activity with structural flexibility in self-supported electrodes remains a pivotal challenge for durable zinc-air batteries (ZABs). Herein, a shallow-etching pyrolysis strategy is proposed to synthesize flexible N/S co-doped carbonized cotton cloth (N/S-CCC) electrodes via hydroxyl-mediated thiourea adsorption. Unlike conventional etching methods that compromise mechanical integrity, this approach achieves controlled surface activation while generating self-adaptive N/S species and mechanical flexibility. The optimized N/S-CCC-2 electrode exhibits synergistic heteroatom interactions between pyridinic-N (electron density regulation) and thiophene-S (spin-state modulation), reducing the rate-determining step energies to 0.75 eV for ORR and 0.85 eV for OER. With an ultrahigh surface area (1230 m 2 ·g −1 ) and minimized strain, the catalyst exhibits outstanding bifunctional oxygen activity (ΔE = 0.78 V in 0.1 mol·L −1 KOH), ranking it among the top-tier metal-free catalysts. When employed into aqueous ZABs, the N/S-CCC-2 electrode delivers a peak power density of 255 mW·cm −2 and ultra-stable cycling over 1000 h. Flexible ZABs further demonstrate mechanical robustness (400 bending cycles) with minimal performance decay, outperforming traditional slurry-coated Pt/C + RuO 2 counterparts. This work establishes a sustainable, metal-free, binder-free paradigm to resolve the catalytic activity-flexibility trade-off in energy storage devices.

CAS / MDL: 110-26-9 62-56-6
研究领域: 材料科学 · 能源存储技术
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2025 · IF 14.3

P2/P3 Biphasic layered oxide cathode enabled by additional electron-holes on oxygen for high-capacity sodium-ion batteries

Hassan Muhammad Mudassir,Chenghao Xie,Fanjie Xia,Rui Fang,Qiushuang Chen,Zhaopei Liu,Tiancheng Dong,Fang Liu,Shan Hu,Zelang Jian,Jinsong Wu

Layered transition metal (TM) oxides have gained significant attention for achieving high specific capacity and energy density utilizing the lattice oxygen redox for sodium-ion batteries. However, the highly oxidized lattice oxygen cannot be fully reduced due to irreversible structural deformation, phase transition, and sluggish kinetics. Herein, the Cobalt (Co) content was tuned to synthesize a P2/P3- biphasic layered oxide cathode Na 0.72 Li 0.24 Co 0.12 Mn 0.64 O 2 (NLM-Co12%), which exhibits pronounced lattice oxygen activity, leading to exceptional capacity and improved cyclability with superior structural stability. The distinct honeycomb ordering induces highly delocalized π-type interactions that generate additional electron holes on oxygen, providing a record energy density and specific capacity of 767.98 Wh kg −1 and 287.19 mAh g −1 , respectively. The strategic incorporation of Co in the TM layers mitigates the sluggish kinetics during the electrochemical reactions and improves the diffusion kinetics. The addition of electron holes on Oxygen (O) is comprehensively investigated through different electrochemical and state-of-the-art spectroscopic techniques. Furthermore, in situ-XRD reveals the phase transition during Na + insertion/extraction is eliminated due to the synergistic effect of the P2/P3 biphasic structure achieving superior structural stability. Benefiting from the superstructure ordering and P2/P3 biphasic structure, the NLM-Co12% electrode demonstrates simultaneously high lattice-oxygen activity and excellent structural stability, thus resulting in remarkable energy density and specific capacity.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Improved activity of oxygen in Ni–Ce0.8Sm0.2O2-δ anode for solid oxide fuel cell with Pr doping

Zhiyong Huang,Lijun Fan,Nianjun Hou,Tian Gan,Juanjuan Gan,Yicheng Zhao,Yongdan Li

Ni–Ce 0.8 Pr x Sm 0.2-x O 2-δ (x = 0–0.15) is studied as an anode of solid oxide fuel cells. The doping of Pr facilitates the chemical oxidation of CH 3 OH on the ceramic phase because the strength of Pr–O bond is weaker than that of Ce–O bond. With the addition of Pr, the electronic conductivity of the ceramic phase increases in an oxidizing atmosphere but decreases in a reducing atmosphere. The electrochemical conductivity relaxation results indicate that Pr improves oxygen surface exchange coefficient and oxygen chemical diffusion coefficient of Ce 0.8 Sm 0.2 O 2-δ simultaneously. The doping of Pr shows negligible influence on the performance of the cell fed with H 2 due to the high reactivity of H 2 . However, the maximum power density of the cell with methanol as the fuel increases significantly with the addition of Pr in the anode, demonstrating the high importance of the oxygen activity of the anode when a less active fuel is used. A Ce 0.8 Sm 0.2 O 2-δ -carbonate electrolyte-supported single cell with Ni–Ce 0.8 Pr 0.1 Sm 0.1 O 2-δ anode shows a maximum power density of 792 mW cm −2 at 650 °C with methanol as the fuel.

研究领域: 材料科学 · 能源科学
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Journal of Cleaner Production · 2023 · IF 11.1

Anaerobic co-metabolic degradation of ceftriaxone sodium: Performance and mechanism

Haoran Chen,Zongping Wang,Yuxin Huang,Junchi Wei,Gang Guo,Lei Miao

Ceftriaxone sodium (CTX) is a typical β-lactam antibiotic in pharmaceutical wastewater. Although traditional biological treatments are low-cost and eco-friendly, antibiotics usually inhibit microorganisms , resulting in limited treatment performance. The biological co-metabolism process provides carbon sources and energy for microorganisms through co-substrate addition, thereby producing enzymes or cofactors to enhance the degradation of refractory pollutants. Therefore, the present study aimed to investigate the degradation performance of CTX through anaerobic biological co-metabolism. A simple co-metabolic substrate (i.e., glucose, 80 mg L −1 ) was added into an anaerobic-activated sludge system, and its mechanism was explored in terms of the variations in extracellular polymeric substances , microbial structure, and resistance genes. Additionally, the possible degradation pathways of CTX were described. The results showed that the degradation efficiency of CTX (200 mg L −1 ) was only about 35% within 8 h in the control group, while it increased to 67.6% in the experimental group with glucose. Chloroflexi , Actinobacteria , Bacteroidetes ADurb.Bin123, and Bacteroidales were the predominant bacterial species in the system. Additionally, the types of enzymes and the relative abundance of β-lactam resistance genes in the co-metabolic system significantly increased by 7 and 0.77%, respectively. Furthermore, nine primary anaerobic CTX biodegradation products were detected, indicating the existence of three possible degradation pathways. Overall, the study results provide a novel approach to treating CTX-containing wastewater.

CAS / MDL: 104376-79-6 50-99-7
研究领域: 环境科学 · 微生物学
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CHEMICAL ENGINEERING SCIENCE · 2023 · IF 4.7

Oxygen activity regulation over LaNiO3 perovskites by Ti substitution for chemical looping partial oxidation of methane

Xian Yao,Xianhua Zhang,Rui Liu,Chunlei Pei,Zhi-Jian Zhao,Jinlong Gong

The oxygen species in oxygen carriers directly influence the reaction performance in chemical looping processes. This paper describes the relationship between oxygen species and performance in chemical looping partial oxidation of methane (CLPOM) over LaNi x Ti 1- x O 3- δ ( x  = 0, 0.25, 0.5, 0.75 and 1) perovskites . Due to the increase of Ti substitution, the predominate reaction during CLPOM gradually changes from complete oxidation to partial oxidation. Quasi in situ XPS characterization suggests that the relative concentration of nucleophilic lattice oxygen species for partial oxidation increases with Ti substitution, while the relative concentration of electrophilic adsorbed oxygen species for complete oxidation decreases. The moderate Ti substitution for LaNi 0.5 Ti 0.5 O 3- δ provides the suitable lattice oxygen activity for the methane partial oxidation. Moreover, LaNi 0.5 Ti 0.5 O 3- δ exhibits high cyclic stability in redox cycles. This work demonstrates that the regulation of oxygen species distribution and activity is feasible to tailor the reaction performance of oxygen carriers in chemical looping processes.

研究领域: 材料科学 · 化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Boosting performance of Co-free Li-rich cathode material through regulating the anionic activity by means of the strong TaO bonding

Chao Wu,Heng Li,Shuang Cao,Zhi Li,Peng Zeng,Jiarui Chen,Xitong Zhu,Xiaowei Guo,Gairong Chen,Baobao Chang,Yongqiang Shen,Xianyou Wang

Benefiting from the extra contribution of O redox, Co-free Li-rich layered oxides (LRNMO) can satisfy the requirement of high specific capacities. However, during the high-voltage charging process, lattice oxygen being oxidized to O − or O 2 leads to a gradual transition of the structure from layered to spinel phase, capacity and voltage decline, hindering the practical application of LRNMO in the lithium-ion battery. Here, a surface modification strategy of Li 1.2 Ni 0.32 Mn 0.48 O 2-δ doped with Ta 5+ ions is proposed, in which the Ta 5+ ions occupy the lithium sites of the lattice structure on the surface layer of LRNMO and form a Ta 2 O 5 coating layer. The modified electrode exhibits excellent rate performance and cycling stability, with 94.9% and 85.5% capacity retention rate and voltage retention rate, respectively, after 200 cycles at 1C. Moreover, the initial coulomb efficiency and ionic conductivity of the modified electrode are also apparently enhanced. Simultaneously, the decreased Li/Ni mixing degree of the modified electrode reflects the improvement of the structural stability . Therefore, the modification strategy through strong metal–oxygen bonding to integrate the surface structure to regulate the oxygen activity provides a new direction for the design of high energy density Co-free Li-rich cathode materials .

研究领域: 材料科学 · 电化学
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