INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Jun Zhu,Jun Chen,Jianan Chen,Jicheng Zhou,Wentao Xu
Direct decomposition of H 2 S into H 2 and S is an attractive alternative to the Claus process, because CO x -free H 2 and S can be simultaneously recovered from an abundant and toxic waste gas, which has huge social economic and ecological environmental benefits. However, it is still a great challenge to achieve the direct H 2 S decomposition reaction with high efficiency due to the thermal equilibrium limitation. Herein, a core-shell structured Mo x C@ZrO 2 was developed as novel microwave catalyst for microwave catalytic H 2 S decomposition. More specifically, the H 2 S conversion over Mo x C@ZrO 2 catalyst is as high as 99.9% at 650 °C, which immensely surpasses the H 2 S equilibrium conversion (6.1% at 650 °C). This study provides an effective strategy for the design of highly active microwave catalysts, and supplies a strategy for efficiently catalytic decomposition of H 2 S waste and recovering high-value hydrogen and sulfur at lower reaction temperatures.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Ziqiang Wang,Guanghui Yang,Pengjun Tian,Xinmiao Li,Kai Deng,Hongjie Yu,You Xu,Hongjing Wang,Liang Wang
The use of thermodynamically more favorable sulfion oxidation reaction (SOR) to replace sluggish oxygen evolution reaction is an effective method for energy-saving production of hydrogen. Herein, we propose the synthesis of organic–inorganic hybrid through the modification of 1-hydroxyethylidene-1,1-diphosphonic acid on Rh metallene (HEDP-Rh metallene) as a bifunctional electrocatalyst for hydrogen evolution reaction (HER) and SOR. The modification of hydrophilic HEDP can effectively promote the water adsorption, thereby accelerating the mass/electron transfer at the interface. The HEDP-Rh metallene requires low overpotentials of 30 mV at 10 mA cm −2 for HER and 0.538 V at 100 mA cm −2 for SOR. In HER-SOR coupled reaction, HEDP-Rh metallene drives the current density of 100 mA cm −2 at 1.08 V for concurrent production of hydrogen and sulfur, highlighting energy-efficient hydrogen production and sulfur recycle.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
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IF 7.8
Junyun Cheng,Chenruobing Zhang,Jie Lin,Yeqiu Zhao,Yu Huang,Meiqing Shi,Zhiqi Zhu,Liyuan Chai,Xu Yan,Qingwei Wang
The coking industry generates hazardous desulfurization waste liquid (DWL), which contains abundant sulfur-containing salts such as ammonium thiocyanate (AT), ammonium sulfate (AS), and ammonium thiosulfate. However, improper handling of DWL poses severe environmental risks. Conventional treatment methods, including high-temperature pyrolysis, chemical precipitation, and evaporation crystallization, suffer from critical limitations: low sulfur recovery rates (typically 40%–70%), high operational costs, and insufficient product purity. To address these challenges, this study innovatively proposes an evaporation-cooling pretreatment process guided by the NH₄SCN-AS-H₂O ternary phase equilibrium system. For the first time, this method achieves ultra-high-purity products: ammonium thiocyanate (AT) at 98.54% purity and ammonium sulfate (AS) at 99.92% purity, with a total sulfur recovery rate of 90.92%—40% higher than traditional approaches. Additionally, the mixed salt (MS) byproduct undergoes solvent crystallization to yield secondary products with purity exceeding 99.96%, eliminating the need for toxic reagents. By integrating phase diagram-guided optimization with streamlined operational procedures, this process significantly reduces costs while ensuring environmental sustainability, thereby establishing a novel pathway for resource recovery from DWL.
研究领域:
环境工程
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化工技术
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资源回收
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DOI
高影响因子
ACS Applied Nano Materials
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2023
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IF 5.9
Hongjing Wang,Beibei Wang,Hongjie Yu,Kai Deng,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
Electrocatalytic water splitting is an important approach for sustainable and green production of hydrogen but is greatly hampered by the sluggish oxygen evolution reaction (OER). Therefore, developing a favorable alternative reaction to replace OER for both energy-efficient coproduction of hydrogen and value-added chemicals is highly desirable. Herein, a thermodynamically favorable sulfion oxidation reaction (SOR) electrocatalyzed by CoNi2S4 nanoflowers (CoNi2S4 NFs) is reported to couple with the hydrogen evolution reaction (HER) for energy-efficient hydrogen production and sulfur recovery. In this coupled system, only a low cell voltage of 0.3 V is required to produce hydrogen at 10 mA cm–2, much lower than that of water splitting (1.76 V). Meanwhile, S2– ions are selectively electrooxidized to sulfur with a high yield of 220.5 g h–1 m–2, realizing electrochemical upcycling of sulfur-containing pollutants. This strategy provides an attractive route for both energy-effective hydrogen generation and sulfur recycling.
研究领域:
能源化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Jiali Zhang,Dapeng Li,Yujing Weng,Qi Sun,Sebastien A. Duval,Rashid M. Al Othman,George P. Lithoxoos,Yulong Zhang
Due to stricter worldwide environmental mandates on SO2 emission from oil and gas industrial facilities, the modified Claus process, which is the primary tool for reducing emission of SO2 into the atmosphere in these facilities, has undergone a lot of innovative changes during the past decades. An example of such innovation is the addition of what is called tail gas treating (TGT) technologies. Currently, advanced TGT technologies ensure that gas plants and refineries emit less than 0.01% (v/v) of the sulfur species that enter into the sulfur recovery units; they commonly use absorption-based processes to separate sulfur species from the tail gas. Because of this requirement, TGT technologies are expensive. This paper reports the data that were obtained from bench-scale tests that were carried out to assess the feasibility of using commercially available adsorbents for the process that is described in the patent, Two-Stage Adsorption Process for Claus Tail Gas Treatment, US Patent No.10662061. In one of the embodiments of this process, the tail gas is treated in two steps. It is first dehydrated by 3A molecular sieves and then by 5A molecular sieves to remove H2S. The separation in the second step will ensure the presence of a rich H2S-laden stream that is ready for routing to the thermal reactor of the modified Claus process. The data collected in this study indicate the following: (1) Commercial molecular sieves can be used for cost-effective tail gas treatment of natural gas plants’ and refineries’ sulfur recovery units. (2) This cost-effectiveness of such use can be valid when molecular sieve material selection is as described in US Patent No.10662061, “Two-Stage Adsorption Process for Claus Tail Gas Treatment”. (3) Adsorption-based tail gas treatment is advantageous since it results in enabling the global oil and gas industry to virtually eliminate all SO2 emissions from its facilities.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
Sustainable Energy & Fuels
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2025
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IF 4.1
Zihang Yu,Weiguang Ma,Enqing Xue,Yuening Ma,Yichen Zhang,Yuan Haofu,Yupeng Xiao,Hefeng Zhang,Xu Zong
The valorization of hydrogen sulfide (H₂S) through its dissociation into hydrogen and elemental sulfur presents a promising route for converting hazardous waste into valuable commodities. Here, we report a novel redox flow battery (RFB) system employing polyoxometalate-based redox couples that achieves highly efficient H₂S conversion. The anodic H₅[PMo₂VMo₁₀VIO₄₀]/H₃[PMo₁₂VIO₄₀] system demonstrates three critical advantages over conventional Fe²⁺/Fe³⁺ mediators: (1) minimal membrane crossover, (2) high volumetric capacity (more than 3.5 times), and (3) rapid reaction kinetics (k₀ = 0.022 cm s⁻¹). When coupled with the cathodic H₄[SiW₁₂VIO₄₀]/H₆[SiW₁₀VIW₂VO₄₀] system, this design demonstrates 90% faradaic efficiency for simultaneous H₂ and sulfur production. The synergistic combination of these redox mediators establishes a sustainable platform for toxic H₂S conversion while enabling scalable hydrogen production and sulfur recovery.
研究领域:
化学工程
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能源科学
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环境科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jiayu Feng,Lijuan Jia,Fei Wang,Xin Sun,Ping Ning,Chi Wang,Yuan Li,Kai Li
In this work, we report a novel urea-modified copper-based material (XUrea@Cu) obtained by directly calcinating a mixture of urea and copper nitrate. This material enables the efficient purification of H 2 S under dry and anaerobic conditions. The performance test results showed that the H 2 S capacity of the optimal adsorbent (2Urea@Cu) could reach 364.2 mg(H 2 S)∙g sorbent -1 , which is much superior to those of other adsorbents in the literature. Further study demonstrates that the ultra-desulfurization performance of 2Urea@Cu is mainly attributed to the extensive alkaline site, the high concentrations of active oxygen, and the abundance of oxygen vacancy; which are quite effective for capturing H 2 S (acidic and strong reducibility). Interestingly, the deactivation adsorbent (De-2Urea@Cu) is mainly composed of high-purity CuS, which means that the Urea@Cu adsorbent can simultaneously achieve efficient purification of H 2 S and recovery of sulfur resources since CuS is a valuable product. In addition, in-situ FT-IR and theoretical calculation results indicate that H 2 S molecules dissociate on the CuO(1 1 1) surface by stepwise dehydrogenation, while S combines with adjacent Cu to form CuS. The consumption of active components (CuO) and the accumulation of reaction products (CuS) are the primary reasons for the deactivation of adsorbents. Considering the simple preparation process, low cost, and excellent H 2 S adsorption activity, these urea-modified copper-based materials are very promising H 2 S adsorbents.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Fanyun Chen,Chen Tian,Xuelin Pan,Qingshan Gao,Qingwei Wang,Liyuan Chai,Zhang Lin
Metallurgical sulfur-containing wastes (MSCWs) is an important secondary resource for recovering element sulfur in chemical and metallurgical industries. However, it is challenging to simultaneously achieve high recovery rate and sulfur purity, due to the multiple impurities combining with sulfur in these wastes. In this paper, we developed a novel method of pressure induced melting-crystallization to efficiently recover sulfur from MSCWs. The effects of condition parameters on the sulfur recovery rate and purity were optimized through response surface methodology. The single objective optimization results showed that the interaction between melting temperature and slurry concentration had a great influence on sulfur purity. The slurry concentration and pressure had great influence on sulfur recovery rate. The results of multi-objective optimization showed that under the conditions of pressure 1.2 MPa, slurry concentration 14.9% and melting temperature 140.9℃, the highest sulfur purity and recovery rate could reach 93.0% and 89.1% respectively. Mechanism investigation revealed that the high efficiency of sulfur recovery was ascribed to recrystallization of molten sulfur under the combined action of pressure and water, forming dense sulfur blocks and separating hydrophilic impurities. This work provides a new way to recover sulfur resources from MSCWs with sulfur content higher than 50%.
研究领域:
冶金工程
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环境科学
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化学工程
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Chao Duan,Chun Tang,Yonghong Du,Shan Yu,Heng Guo,Yu Bai,Ying Zhou
Solar-driven electrochemical dissociation of hydrogen sulfide (H 2 S) to hydrogen and sulfur products in photovoltaic-electrochemical (PV-EC) devices becomes an effective strategy for acid gas purification and energy-saving hydrogen production . However, available H 2 S splitting electrochemical devices suffer from inferior energy conversion efficiency and fussy multi-step sulfur recovery problems. Herein, we propose an integrated solar-driven PV-EC system with diaphragm electrolytic reactor to solve these challenges. The optimized system integrated commercial silicon solar delivers a high solar-to-hydrogen energy conversion efficiency of up to 12 %, with approximately 99 % H 2 faradaic efficiency and demonstrates at least 50 hours of stability. More importantly, the S 2- /HS - can be transformed into add-valued Na 2 S 2 O 3 by one-step method in Na 2 SO 3 media, which avoids complex sulfur recovery. This work presents an alternative method of low-energy consumption for producing H 2 and high-value sulfur-related chemicals by H 2 S splitting through a PV-EC system.
研究领域:
能源科学
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电化学工程
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环境科学
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Jiaxin Li,Chongchao Yao,Bo Song,Zhihao Zhang,Andreas Libonati Brock,Stefan Trapp,Jing Zhang
Microbial fuel cells (MFCs) have great promise for power generation by oxidizing organic wastewater, yet the challenge to realize high efficiency in simultaneous energy production and resource recovery remains. In this study, we designed a novel MFC anode by synthesizing S-doped NiFe 2 O 4 nanosheet arrays on carbon cloth (S10-NiFe 2 O 4 @CC) to build a three-dimensional (3D) hierarchically porous structure, with the aim to regulate the microbial community of sulfur-cycling microbes in order to enhance power production and elemental sulfur (S 0 ) recovery. The S10-NiFe 2 O 4 @CC anode obtained a faster start-up time of 2 d and the highest power density of 4.5 W/m 2 in acetate-fed and mixed bacteria-based MFCs. More importantly, sulfide removal efficiency (98.3 %) (initial concentration of 50 mg/L S 2− ) could be achieved within 3 d and sulfur (S 8 ) could be produced. Microbial community analysis revealed that the S10-NiFe 2 O 4 @CC anode markedly enriched sulfur-oxidizing bacteria (SOB) and promoted enrichment of SOB and sulfate-reducing bacteria (SRB) in the bulk solution as well, leading to the enhancement of power generation and S 0 recovery. This study shows how carefully designing and optimizing the composition and structure of the anode can lead to the enrichment of a multifunctional microbiota with excellent potential for sulfide removal and resource recovery.
研究领域:
环境工程
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微生物学
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能源技术
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Xiaoqiong Hao,Qian Yang,Xiaotong Zhuo,Shiyuan Zhou,Danfeng Wang,Ye Zhang,Guangfeng Liu,Yingjie Liu,Peiyang Gu
This study introduces a self-driven system that effectively achieves synchronized sulfur recovery and hydrogen production using a Zn-air battery. The system ingeniously integrates the sulfur oxidation reaction (SOR) and the hydrogen evolution reaction (HER) into a single, efficient process. Central to this system is the trifunctional phosphorus-doped cobalt molybdate catalyst (P-CoMoO 4 /NF), which exhibits superior performance in both HER (η j = 100 = 0.13 V) and SOR (η j = 100 = 0.30 V) with remarkable stability (∼360 h), reaching 0.64 V at 100 mA cm −2 for simultaneous sulfur ion degradation and hydrogen production . Through density functional theory simulations and extensive characterizations, it has been shown that phosphorus doping in the cobalt molybdate catalyst facilitates electron redistribution, enhancing the catalyst's conductivity, generating more oxygen vacancies, and promoting improved mass and electron transfer. This modification also lowers the energy barrier for adsorbing reaction intermediates, thus increasing the hydrogen production rate and sulfur oxide conversion in this self-powered system. In summary, this research marks a substantial advancement in the development of trifunctional catalysts and proposes an eco-friendly, cost-effective strategy for integrated reaction systems, paving the way for sustainable energy solutions.
研究领域:
能源材料科学
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环境化学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
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2024
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IF 5.2
Jia-tao Xiang,Jun-ting Li,Xiong Zhang,Han Zhang,Shao-hui Ren,Shi-hong Zhang
This study focused on the development of a novel process of H2O2/FeSO4 preoxidation combined with wet flue gas desulfurization (WFGD) postabsorption for simultaneous desulfurization and denitrification, and recovery of sulfur and nitrogen from flue gas. The results show that when no oxidant is added, the denitrification efficiency by WFGD is only 5.3%, while under the H2O2/FeSO4 preoxidation, the desulfurization and denitrification efficiency can reach 99.9% and 83.6%, respectively. When the liquid/gas ratio reaches 18 L·m–3, the desulfurization efficiency is nearly 100%, and the denitrification efficiency can reach 90.6% due to the increased liquid/gas contact area and improved heat and mass transfer. The absorption process of SO2 and NOx involves both physical and chemical absorption, which is dominated by physical absorption, and the absorption characteristics are multilayer absorption. The desulfurization products CaSO3 and CaSO4, and the denitrification products Ca(NO2)2 and Ca(NO3)2, are absorbed by the CaCO3 slurry. The Aspen Plus process simulation results show that the desulfurization and denitrification efficiencies are 99.5% and 89.6%, respectively, and the concentrations of SO2 and NOx in the flue gas are 21.4 mg·m–3 and 41.5 mg·m–3, respectively, which meet the ultralow emission standards. In addition, the H2O2/NO molar ratio, oxidation temperature, and SO2 concentration have an important effect on the NO conversion, which then affects the denitrification efficiency.
研究领域:
环境工程
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化学工程
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过程模拟
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）