煤层气治理与利用技术研究开发进展

煤层气作为一种非常规天然气,既是宝贵的清洁能源,其主要成分甲烷同时也是一种主要的温室气体;煤层气的直接排放不仅加剧了大气温室效应和环境污染,同时也是能源资源的极大浪费.近年来,煤层气的治理和利用受到了广泛关注,有关技术研究和开发取得了很大进展.本文对近年来煤层气的治理和利用技术研发进展进行了总结和评估,侧重于介绍煤层气分离系统中关键的中、高浓度煤层气催化燃烧脱氧技术以及乏风瓦斯逆向流催化燃烧减排及余热利用技术.最后对煤层气综合利用技术进行了展望.     

Carbon dioxide capture-related gas adsorption and separation in metal-organic frameworks

Reducing anthropogenic CO₂ emission and lowering the concentration of greenhouse gases in the atmosphere has quickly become one of the most urgent environmental issues of our age. Carbon capture and storage (CCS) is one option for reducing these harmful CO₂ emissions. While a variety of technologies and methods have been developed, the separation of CO₂ from gas streams is still a critical issue. Apart from establishing new techniques, the exploration of capture materials with high separation performance and low capital cost are of paramount importance. Metal-organic frameworks (MOFs), a new class of crystalline porous materials constructed by metal-containing nodes bonded to organic bridging ligands hold great potential as adsorbents or membrane materials in gas separation. In this paper, we review the research progress (from experimental results to molecular simulations) in MOFs for CO₂ adsorption, storage, and separations (adsorptive separation and membrane-based separation) that are directly related to CO₂ capture.     

Electrocatalytic Recycling of CO2 and Small Organic Molecules

As global warming directly affects the ecosystems and humankind in the 21^st century, attention and efforts are continuously being made to reduce the emission of greenhouse gases, especially carbon dioxide (CO₂). In addition, there have been numerous efforts to electrochemically convert CO₂ gas to small organic molecules (SOMs) and vice versa. Herein, we highlight recent advances made in the electrocatalytic recycling of CO₂ and SOMs including (i) the overall trend of research activities made in this area, (ii) the relations between reduction conditions and products in the aqueous phase, (iii) the challenges in the use of gas diffusion electrodes for the continuous gas phase CO₂ reduction, as well as (iv) the development of state of the art hybrid techniques for industrial applications. Perspectives geared to fully exploit the potential of zero‐gap cells for CO₂ reduction in the gaseous phase and the high applicability on a large scale are also presented. We envision that the hybrid system for CO₂ reduction supported by sustainable solar, wind, and geothermal energies and waste heat will provide a long term reduction of greenhouse gas emissions and will allow for continued use of the abundant fossil fuels by industries and/or power plants but with zero emissions.     

Adsorption technology for CO2 separation and capture: a perspective

The capture of CO₂ from process and flue gas streams and subsequent sequestration was first proposed as a greenhouse gas mitigation option in the 1990s. This proposal spawned a series of laboratory and field tests in CO₂ capture which has now grown into a major world-wide research effort encompassing a myriad of capture technologies and ingenious flow sheets integrating power production and carbon capture. Simultaneously, the explosive growth in materials science in the last two decades has produced a wealth of new materials and knowledge providing us with new avenues to explore to fine tune CO₂ adsorption and selectivity. Laboratory and field studies over the last decade have explored the synergy of process and materials to produce numerous CO₂ capture technologies and materials based on cyclic adsorption processes. In this brief perspective, we look at some of these developments and comment on the application and limitations of adsorption process to CO₂ capture. We identify major engineering obstacles to overcome as well as potential breakthroughs necessary to achieve commercialization of adsorption processes for CO₂ capture. Our perspective is primarily restricted to post-combustion flue gas capture and CO₂ capture from natural gas.     

Engineering of Ruthenium–Iron Oxide Colloidal Heterostructures: Improved Yields in CO2 Hydrogenation to Hydrocarbons

Catalytic CO₂ reduction to fuels and chemicals is a major pursuit in reducing greenhouse gas emissions. One approach utilizes the reverse water‐gas shift reaction, followed by Fischer–Tropsch synthesis, and iron is a well‐known candidate for this process. Some attempts have been made to modify and improve its reactivity, but resulted in limited success. Now, using ruthenium–iron oxide colloidal heterodimers, close contact between the two phases promotes the reduction of iron oxide via a proximal hydrogen spillover effect, leading to the formation of ruthenium–iron core–shell structures active for the reaction at significantly lower temperatures than in bare iron catalysts. Furthermore, by engineering the iron oxide shell thickness, a fourfold increase in hydrocarbon yield is achieved compared to the heterodimers. This work shows how rational design of colloidal heterostructures can result in materials with significantly improved catalytic performance in CO₂ conversion processes.     

Solar Driven Gas Phase Advanced Oxidation Processes for Methane Removal - Challenges and Perspectives

Methane (CH₄) is a potent greenhouse gas and the second highest contributor to global warming. CH₄ emissions are still growing at an alarmingly high pace. To limit global warming to 1.5 °C, one of the most effective strategies is to reduce rapidly the CH₄ emissions by developing large-scale methane removal methods. The purpose of this perspective paper is threefold. (1) To highlight the technology gap dealing with low concentration CH₄ (at many emission sources and in the atmosphere). (2) To analyze the challenges and prospects of solar-driven gas phase advanced oxidation processes for CH₄ removal. And (3) to propose some ideas, which may help to develop solar-driven gas phase advanced oxidation processes and make them deployable at a climate significant scale.     

Emission of Toxic HCN During NOx Removal by Ammonia SCR in the Exhaust of Lean‐Burn Natural Gas Engines

Reducing greenhouse gas and pollutant emissions is one of the most stringent priorities of our society to minimize their dramatic effects on health and environment. Natural gas (NG) engines, in particular at lean conditions, emit less CO₂ in comparison to combustion engines operated with liquid fuels but NG engines still require emission control devices for NO_x removal. Using state‐of‐the‐art technologies for selective catalytic reduction (SCR) of NO_x with NH₃, we evaluated the interplay of the reducing agent NH₃ and formaldehyde, which is always present in the exhaust of NG engines. Our results show that a significant amount of highly toxic hydrogen cyanide (HCN) is formed. All catalysts tested partially convert formaldehyde to HCOOH and CO. Additionally, they form secondary emissions of HCN due to catalytic reactions of formaldehyde and its oxidation intermediates with NH₃. With the present components of the exhaust gas aftertreatment system the HCN emissions are not efficiently converted to non‐polluting gases. The development of more advanced catalyst formulations with improved oxidation activity is mandatory to solve this novel critical issue.     

Sustainability Evaluation of Immobilized Acid-Adapted Microalgal Technology in Acid Mine Drainage Remediation following Emergy and Carbon Footprint Analysis

Sustainability evaluation of wastewater treatment helps to reduce greenhouse gas emissions, as it emphasizes the development of green technologies and optimum resource use rather than the end-of-pipe treatment. The conventional approaches for treating acid mine drainages (AMDs) are efficient; however, they need enormous amounts of energy, making them less sustainable and causing greater environmental concern. We recently demonstrated the potential of immobilized acid-adapted microalgal technology for AMD remediation. Here, this novel approach has been evaluated following emergy and carbon footprint analysis for its sustainability in AMD treatment. Our results showed that imported energy inputs contributed significantly (>90%) to the overall emergy and were much lower than in passive and active treatment systems. The microalgal treatment required 2–15 times more renewable inputs than the other two treatment systems. Additionally, the emergy indices indicated higher environmental loading ratio and lower per cent renewability, suggesting the need for adequate renewable inputs in the immobilized microalgal system. The emergy yield ratio for biodiesel production from the microalgal biomass after AMD treatment was >1.0, which indicates a better emergy return on total emergy spent. Based on greenhouse gas emissions, carbon footprint analysis (CFA), was performed using default emission factors, in accordance with the IPCC standards and the National Greenhouse Energy Reporting (NGER) program of Australia. Interestingly, CFA of acid-adapted microalgal technology revealed significant greenhouse gas emissions due to usage of various construction materials as per IPCC, while SCOPE 2 emissions from purchased electricity were evident as per NGER. Our findings indicate that the immobilized microalgal technology is highly sustainable in AMD treatment, and its potential could be realized further by including solar energy into the overall treatment system.     

Electrochemical CO2 Activation and Valorization on Metallic Copper and Carbon-Embedded N-Coordinated Single Metal MNC Catalysts

The electrochemical reductive valorization of CO₂, referred to as the CO2RR, is an emerging approach for the conversion of CO₂-containing feeds into valuable carbonaceous fuels and chemicals, with potential contributions to carbon capture and use (CCU) for reducing greenhouse gas emissions. Copper surfaces and graphene-embedded, N-coordinated single metal atom (MNC) catalysts exhibit distinctive reactivity, attracting attention as efficient electrocatalysts for CO2RR. This review offers a comparative analysis of CO2RR on copper surfaces and MNC catalysts, highlighting their unique characteristics in terms of CO₂ activation, C₁/C₂₍₊₎ product formation, and the competing hydrogen evolution pathway. The assessment underscores the significance of understanding structure–activity relationships to optimize catalyst design for efficient and selective CO2RR. Examining detailed reaction mechanisms and structure-selectivity patterns, the analysis explores recent insights into changes in the chemical catalyst states, atomic motif rearrangements, and fractal agglomeration, providing essential kinetic information from advanced in/ex situ microscopy/spectroscopy techniques. At the end, this review addresses future challenges and solutions related to today's disconnect between our current molecular understanding of structure–activity-selectivity relations in CO2RR and the relevant factors controlling the performance of CO₂ electrolyzers over longer times, with larger electrode sizes, and at higher current densities.     

Modelling effects of geoengineering options in response to climate change and global warming: Implications for coral reefs

Climate change will have serious effects on the planet and on its ecosystems. Currently, mitigation efforts are proving ineffectual in reducing anthropogenic CO₂ emissions. Coral reefs are the most sensitive ecosystems on the planet to climate change, and here we review modelling a number of geoengineering options, and their potential influence on coral reefs. There are two categories of geoengineering, shortwave solar radiation management and longwave carbon dioxide removal. The first set of techniques only reduce some, but not all, effects of climate change, while possibly creating other problems. They also do not affect CO₂ levels and therefore fail to address the wider effects of rising CO₂, including ocean acidification, important for coral reefs. Solar radiation is important to coral growth and survival, and solar radiation management is not in general appropriate for this ecosystem. Longwave carbon dioxide removal techniques address the root cause of climate change, rising CO₂ concentrations, they have relatively low uncertainties and risks. They are worthy of further research and potential implementation, particularly carbon capture and storage, biochar, and afforestation methods, alongside increased mitigation of atmospheric CO₂ concentrations.     

Hydrothermal synthesis of one-dimensional α-MoO3 nanomaterials and its unique sensing mechanism for ethanol

In gas sensor applications, the availability of highly sensitive and rapid response/recovery detector for ethanol gas is sparse. One-dimensional orthogonal crystalline molybdenum trioxide nanomaterials were synthesized by an economical and environmentally friendly hydrothermal method. X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and energy spectroscopy (EDS) were used to investigate the structure and morphology of the nanometer materials. The relevant characterization shows that nanobelts are highly crystalline layered structures with a width of about 200 nm and a length of a few micrometers. The synthesized ethanol gas sensors based on α-MoO₃ semiconductor material show the highest response at 350 °C. Gas sensitivity tests indicated that α-MoO₃ nanobelts respond well to 50 ～ 600 ppm ethanol at optimal operating temperatures. The selectivity test among various reducing gases shows that the sensor responds better to ethanol compared to other gases such as xylene, NO₂, CO, and H₂ gases. This excellent sensing performance is attributed to the unique sensing mechanism formed in the layered MoO₃ nanobelts through the catalytic reaction between ethanol and MoO₃ lattice oxygen and adsorbed oxygen. The sensing mechanism of the co-catalytic effect of lattice oxygen and adsorbed oxygen on ethanol is also discussed in depth.     

Fluorinated gases for semiconductor manufacture: process advances in chemical vapor deposition chamber cleaning

In the past several years, the semiconductor industry has been presented with various options for cleaning of plasma enhanced chemical vapor deposition (PECVD) tool chambers. In this paper, we assess the relative merits of the latest chamber cleaning processes. These processes will be compared on the overall cleaning performance (process throughput, efficiency of clean) the economic performance (gas usage, costs) and the environmental performance (perfluorocarbon (PFC) emissions). Direct comparisons between chemistries will be made whenever relevant process factors (e.g. tool type, film, analysis methods) are held constant.We have previously reported both laboratory and commercial CVD tool results comparing different chamber cleaning gases. These studies using both Novellus Concept-1 and AMAT P-5000 tools, indicated that a “drop-in” alternative such as octafluorocyclobutane (c-C₄F₈) would significantly lower PFC emissions (up to 85%) as well as decrease process costs through reductions in gas consumption. In this paper, we further extend this work to include qualification and implementation at chipmakers on a variety of tools, wafer sizes, and films. Key process data on film properties such as uniformity, number of particles, and thickness is also presented.The overall results support and extend the basic conclusions reached earlier: c-C₄F₈ has the lowest process cost of any cleaning gas, without any penalty in cleaning performance (process throughput) but most importantly, it also offers the lowest PFC emissions of any fluorocarbon-based process. It is a true drop-in alternative offering the unique win-win combination of improved environmental performance while also reducing processing costs.     

Enhancing the Performance of Evolutionary Algorithm by Differential Evolution for Optimizing Distillation Sequence

Optimal synthesis of distillation sequence is a complex problem in chemical processes engineering, which involves process structure optimization and operation parameters optimization. The study of the synthesis of distillation sequence is a crucial step toward improving the efficiency of chemical processes and reducing greenhouse gas emissions. This work introduced the concept of binary tree to encode the distillation sequence. The performance of the six evolutionary algorithms was evaluated by solving a 14-component distillation sequence synthesis problem. The best algorithm was used to optimize the operation parameters of a triple-column distillation process. The total annual cost and CO₂ emissions were considered as the metrics to evaluate the performance of triple-column distillation processes. As a result, NSGA-II-DE was found to be the best one of the six tested evolutionary algorithms. Then, NSGA-II-DE was applied to the distillation sequence optimization to find the best operating parameters, which led to a significant reduction in CO₂ emission and total annual costs.     

Sulfur impact on diesel emission control- A review

The effect of sulfur on diesel emission control is reviewed in this paper. Diesel exhaust differs from that of petrol engine exhaust in two major characteristics. Firstly, diesel exhaust contains a far higher amount of particulate matter, and secondly, the exhaust is far leaner, that is, far more oxidizing than a typical exhaust from petrol engines. Under these conditions, the conventional three-way catalysts are not effective in reducing NO_x . Emission from diesel engines is a complex phenomenon. The composition, the properties and the amount of these emissions depend on strictly technical parameters such as engine design and engine operation characteristics and on fuel and lube oil composition. Diesel fuel contains a small amount of sulfur which has an adverse effect even on the raw particulate emissions. The investigations on the effect of sulfur on hydrocarbons, CO and NO_x abatement in diesel exhaust gas is reviewed together with the newest technologies to avoid catalyst deactivation by unwanted SO₂ reactions.     

Carbon dioxide fixation by microalgal photosynthesis using actual flue gas from a power plant

Applied Biochemistry and Biotechnology - CO2 fixation by microalgal cultures, a potential method for CO2 emissions mitigation, was studied in small (approx 2 m2) ponds using actual flue gas from...     

光伏太阳能电池生产过程中的污染问题

日益壮大的光伏产业正在为人类发展作出积极的贡献.采用光伏发电来代替传统的发电技术,将会减少89%的空气污染.然而,在这个倡导绿色环境的时代,光伏器件生产引起的环境、健康和安全（EHS）问题也日益引起社会各界的广泛关注.认清光伏产品在生产过程中污染的真相对维持光伏产业的可持续发展有着相当重要的意义.本文综述了常见太阳能电池的EHS问题,并提出了可以减少污染的有效途径;采用生命周期评估（LCA）方法进一步比较了各种太阳能电池生产过程中污染物的排放量数据.     

废水生物脱氮工艺中N2O排放数学模型研究进展

N_2O是一种重要的温室气体,而污水生物脱氮处理过程是N_2O的潜在产生源之一。随着污水处理量和处理程度的不断提高,N_2O的排放量也将不断增大。建立N_2O排放数学模型对污水生物脱氮系统中N_2O生成机制的深入研究和污水处理行业N_2O削减工艺技术的开发具有重大的理论及实践意义。本文归纳了生物脱氮工艺的原理,系统阐述了生物脱氮工艺中N_2O的生成机理和排放数学模型的类型、建立方法及应用情况。在此基础上,对生物脱氮工艺中N_2O排放数学模型的研究现状和研究方向进行了总结和展望,以期为N_2O排放数学模型的完善、N_2O排放量的削减、污水生物脱氮工艺的优化及污水处理行业的可持续发展提供理论基础和科学依据。     

Solubility of methane in pure non-ionic surfactants and pure and mixtures of linear alcohols at 298 K and 101.3 kPa

The emissions of methane (CH₄), a powerful greenhouse gas (GES), contribute to the increase in GES concentration level in the atmosphere. For this reason, the importance of controlling CH₄ emissions of anthropogenic origin has increased over the last decades. Physicochemical and biological processes are available for treating CH₄. For this reason, such properties as the solubility of CH₄ in aqueous solutions and organic solvents are of great relevance in different applications in environmental engineering and biotechnology. In this study, the solubility of CH₄ was determined at 298 K and 101.3 kPa in organic solvents, such as polyoxyethylenesorbates (Tween 20, Tween 40, and Tween 60), and linear alcohols (methanol, ethanol, and butan-1-ol) alone and in their admixtures. Admixtures of methanol with butan-1-ol exhibited the highest solubility of CH₄, of around 0.49 g m⁻³ of solvent, whereas the solubility of CH₄ in linear alcohols varied from 0.167 g m⁻³ to 0.41 g m⁻³ of solvent. In the case of Tweens, CH₄ solubility decreased with the hydrophilic-lipophilic balance (HLB) number.     

In-situ neutron diffraction study of cathode/electrolyte interactions under electrical load and elevated temperature

Fuel cells are proposed as a future energy conversion technology that will reduce greenhouse gas emissions at the point of operation due to their ability to produce electrical energy from non-hydrocarbon fuel sources. The Solid Oxide Fuel Cell (SOFC) is amongst the most efficient fuel cell types, however, due to the high cell operating temperature cation diffusion occurs between the different components of the cell, resulting in rapid degradation of the power output. In this paper we investigate cation migration between the promising intermediate temperature-SOFC cathode La_1−xSr_xCo_1−yFe_yO_3−δ (LSCF) and a fluorite type electrolyte Ce_1−xPr_xO_2−δ (CPO). The crystallographic structure evolution and degradation of the materials were studied by neutron diffraction in-situ under pseudo-operating conditions, i.e. at 600 °C under air and under electrical polarisation. The lattice parameter and cation occupancy evolution were analysed by Rietveld refinement as a function of time and applied potential. The materials were found to be stable, as no impurity formation, lattice parameter or site occupancy evolution was observed during the experiment. However La migration prior to the experiment from LSCF to CPO was observed as well as B-site vacancies in LSCF.