CN1332652A - 利用燃烧副产物未燃烧的炭控制汞的排放 - Google Patents
利用燃烧副产物未燃烧的炭控制汞的排放 Download PDFInfo
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Abstract
通过向烟道气中注入未燃烧的炭来控制自烟道气(例如燃煤发电厂产生的烟道气)的汞的排放,该未燃烧的炭由诸如飞尘或木灰之类的物质提纯得到。未燃烧的炭吸附汞,随后通过粒子分离器从烟道气中除去。与现在应用于该工艺的活性炭相比,自飞尘收集到的未燃烧的炭的费用是非常低的。通过一种或多种用于从飞尘中除去非炭粒子的分离工艺,使得未燃烧的炭在吸附剂中浓缩。这些工艺过程包括重力分离、静电分离、泡沫浮选、磁性分离和粒子大小分类。通过炭表面的氧化可更进一步增加汞的吸附。
Description
发明背景和综述
汞一直被认为是潜在的影响健康和环境的公害。对燃煤发电厂、石油和化学炼厂、煅烧炉、金属萃取操作和其它汞排放设备的环境标准的需求越来越高。现在新的规则章程处于发展当中，以便降低来自上述设备的可允许的汞排放水平。为了迎接这样的挑战，科学技术也处于发展之中。一种技术是利用活性炭来控制自燃煤发电厂产生的汞排放。但是，费用评估表明，该种技术的商业化将导致用电价格增长5％，并且该增长的95％是由于活性炭的费用。
本发明的一个目的是找到较低费用的炭材料，以用于控制汞的排放。我们的研究已经揭示，飞尘、木灰和其它炭化的含炭材料中或来自飞尘的、木灰和其它炭化的含炭材料中的未燃烧的炭是汞的有效吸收剂。这些炭资源在此将被统一称作“飞尘”。这些炭可用作活性炭的替代物。与活性炭相比，来自飞尘中的未燃烧的炭因其通常作为副产物燃烧而很便宜。虽然飞尘可能仅含有很少部分的炭，但是将飞尘升级到较高炭含量的技术费用是有效的。炭的表面处理(例如表面氧化)也将提高其对汞的吸附能力。
我们已经发现，未燃烧的炭具有类似于或者比活性炭更高的吸附能力。其原因可能在于炭的孔结构和汞的吸附特性。例如在活性炭的注入系统中，干燥的活性炭被来自空气压缩机的高速空气载带，并喷雾到烟道气管中，即微粒收集装置的上游。据报道，炭的注入速率是汞排放速率的1000-10000倍，烟道气中炭浓度为30-80mg/m3。在炭的注入排放控制系统中影响炭性能的因素包括温度、相对湿度、汞浓度和烟道气的其它组分。在吸附过程中，炭-汞接触时间非常短，并且很难达到吸附平衡。据估计，由于活性炭中的许多孔是微孔(即小于2纳米)，活性炭因扩散控制而很少有机会吸附汞。结果，活性炭潜在的吸附能力不能有效地利用。
对于未燃烧的炭，孔的大多数是大孔(即大于50纳米)。尽管这些炭与活性炭相比具有很低的表面积(例如一种飞尘炭的表面积为15-200m2/g，许多活性炭的表面积为500-1000m2/g)，但是在炭的注入系统中它们可能和商用的活性炭一样有效地吸附汞。在显示大孔比微孔更加重要，而且需要最小的吸附剂/气体比率。最小的固体/气体比率通常保证吸附物分子(在此为汞)在气相中有适当的机会和吸附剂粒子碰撞。
与活性炭相比，一般来说具有适当的吸附能力的未燃烧的炭的费用较低。未燃烧的炭有更多的大孔，其允许快速吸附和负载后易再生。而且，未燃烧的炭中存在的微量和较少的元素或化合物可能提高汞的吸附能力。用未燃烧的炭来除去汞的最初应用是用在来自燃煤发电厂的烟道气中。但是，它也可用于除去来自煅烧炉烟道气、天然气和氯-碱工艺过程的通风空气中的汞。
结合附图，下面的说明和后附的权利要求将使本发明的其它目的、特点和优点将变得更加明显。
附图简述
图1是比较在未燃烧的炭上和在活性炭上汞吸附的曲线图；
图2是比较在未燃烧的炭上汞吸附的曲线图，该炭是通过两种不同的工艺过程、自飞尘得到的；
图3是表示未燃烧的炭的热氧化对汞吸附的影响因素的曲线图；
图4是阐明在氮气中加热温度对负载了汞的未燃烧的炭的再生作用影响的条形图；
图5是阐明在空气中加热温度对负载了汞的未燃烧的炭的再生作用影响的条形图；
图6是比较未燃烧的炭和再生后的未燃烧的炭之间的汞吸附的曲线图；和
图7是从烟道气流中除去汞的工艺过程的流程图。
优选实施例的详细描述
有许多未燃烧的炭，包括那些飞尘、木灰和其它炭化的含炭材料中或来自飞尘、木灰和其它炭化的含炭材料。这些炭因不包括活化过程而不同于活性炭。因此，需要制备未燃烧的炭来有效吸附汞。制备可以包括使用各种物理和化学分离工艺过程及其结合。这些工艺过程包括筛网、重力(密度)分离；使更具有传导性的炭从飞尘和硅酸盐矿物中分离出来，或通过摩擦电产生不同电荷的静电或摩擦电分离；描述在美国专利US5,047,145中(在此作为参考)的泡沫浮选法除去汞；磁性分离除去铁粒子；粒子大小分类，使细的飞尘粒子与粗糙的炭分开等等。例如，单级湿法精选法可将飞尘中未燃烧的+100目炭升级，使之从30％LOI(烧失量)升级到大于60％LOI。静电分离可进一步将这些炭升级到80％LOI或更高。在另一个实施例中，通过三级泡沫浮选法可使未燃烧的炭含量从2.5％LOI升级到65％LOI。通过再一次的三级泡沫浮选之后，经轻微研磨浓缩物可进一步升级到85％LOI。
图1表示自飞尘源回收的未燃烧的炭的吸附能力。通过重力和静电分离使得含炭量升级(不包括化学分离)。为了进行比较，商业用活性炭的吸附能力(BPL)也包括在图1中。可以看出在较低的汞浓度(5-250μg/m3，对应于燃煤发电厂的烟道气中的汞)时，未燃烧的炭比活性炭具有更高的吸附能力。未燃烧的炭的吸附能力高达在5μg/m3时为50μg/g，在280μg/m3的汞浓度条件下为70μg/g。在相同的条件下，活性炭的吸附能力分别仅有10-50μg/g。
图2表示通过不同回收过程自飞尘净化得到的未燃烧的炭的吸附能力。未燃烧的炭来自相同的飞尘源，但是通过不同的分离过程进行升级。未燃烧的炭-GE通过重力和静电分离过程进行升级。未燃烧的炭-F是通过使用浮选试剂进行泡沫浮选升级的。可以看出曲线的形状基本上相同，并且吸附能力大约相同。这表明在炭表面残留的浮选试剂没有妨碍汞吸附，因此未燃烧的炭的吸附能力没有通过制备方法而显著地改变。
通过未燃烧的炭表面的氧化可提高炭的汞吸附。在炭表面富含氧的位置被认为是从周围环境俘获汞的活性位。支持这一现象的解释是，这些氧基团将跟汞反应形成氧化汞，氧化汞是热力学有利的。通过各种技术可实现未燃烧的炭表面氧的富集，该技术包括在不同温度在富含氧气的气氛中的热氧化、利用各种化学物质的化学氧化(例如硝酸、氯、碘、臭氧、含铁的盐)和其它方法。图3描述了，通过表面热氧化可提高在未燃烧的炭上的汞吸附的效果。未燃烧的炭来自飞尘并通过泡沫浮选升级。氧化的未燃烧的炭来自同样的资源，但是在400℃的空气中热氧化。当未燃烧的炭在此温度下热氧化时，吸附能力提高了四倍。在300℃或高于300℃时发生显著的改进。这种能力提高的原因被认为是归功于在炭表面氧基团的增加。
炭可以放置在烟道气流经的固定床上。但是，炭最有可能直接注入到烟道气流中。如果直接在微粒收集装置的上游注入，炭将随着烟道气中的飞尘除去。收集到的飞尘和炭被送于从飞尘中分离炭。然后炭经再生作用来回收汞。然后再生的炭重新注入到烟道气流中。
将飞尘从烟道气中除去后也可注入炭。这将需要另一个微粒收集装置，但是收集的炭将不能在再生和重新注入到烟道气之前从飞尘中分离出来。可以使用许多微粒收集装置，例如那些传统的用于从燃煤工厂的烟道气中除去飞尘粒子的装置。
图7表示这种系统的一个概念性流程图，其在微粒分离器的上游注入炭。该系统包括从飞尘中分离负载汞的炭、再生分离后的炭并回收汞、以及将炭黑重新注入到烟道气中。
通过加热和湿法冶金的方法可使得汞解吸来再生炭。图4和5分别描述了在氮气中和空气中未燃烧的炭的再生能力。未燃烧的炭首先以与吸附实验相同的方式负载汞。生成的炭中具有的汞浓度为18,000ppb。在吸附实验中，负载汞的炭放置在实验室中的马福炉中，使用氮气或空气来控制气氛。从图4和5可以看出，在400℃的温度下、在氮气中(图4)或空气中(图5)，负载了汞的炭可全部再生。吸附后的汞含量大约是5ppb。表示在这些图中的再生和温度的依赖关系说明汞的吸附在本质上是物理的和化学的吸附。在较低的再生温度下，只有物理吸附的汞可以解吸。化学吸附的汞直到温度接近于汞的沸点时才会解吸。在解吸过程中降低压力将导致解吸需要的温度降低。
图6描述了再生后未燃烧的炭的可重用性。在空气中在400℃的温度下可进行再生作用。未燃烧的炭是一种通过重力和静电分离升级的飞尘炭。在研究的汞浓度范围内，再生后的未燃烧的炭的吸附能力接近于初始的未燃烧的炭：只是稍微低一点。这表明未燃烧的炭经再生后可重复用于吸附。
应该理解，本发明并不只局限于上面列举的和描述的那些，在没有偏离本发明的主旨和下面的权利要求定义的范围内，可以进行各种变化和改进。
Claims (14)
1.一种利用自飞尘中收集的未燃烧的炭、从烟道气流中除去汞蒸汽的方法，其包括步骤：
通过从飞尘中分离一部分非炭粒子来制备炭吸附剂，使得该吸附剂比最初的飞尘具有更大的未燃烧的炭浓度；
随后将炭吸附剂加入到烟道气流中，吸附剂中的未燃烧的炭将烟道气流中的汞吸附；和
随后从烟道气流中收集负载了汞的炭吸附剂。
2.权利要求1的方法，还包括在升温下使吸附剂中未燃烧的炭的表面氧化的步骤。
3.权利要求2的方法，其中未燃烧的炭表面的氧化是在大于300℃的温度下进行。
4.权利要求2的方法，其中未燃烧的炭表面的氧化是在大于400℃的温度下进行。
5.权利要求1的方法，还包括使负载了汞的炭吸附剂的再生步骤，该步骤包括，加热炭吸附剂以除去在其上富集的汞；和将再生了的炭吸附剂加入到烟道气流中。
6.权利要求5的方法，其中将吸附剂加热到约300℃或更高的温度下进行再生。
7.权利要求5的方法，其中将吸附剂加热到约400℃或更高的温度下在空气中进行再生。
8.权利要求5的方法，其中将吸附剂在氮气气氛中加热进行再生。
9.权利要求1的方法，其中在吸附剂中未燃烧的炭粒子的表面积为15-200m2/g。
10.权利要求1的方法，其中分离工艺将使得吸附剂具有至少60％的烧失量(LOI)。
11.权利要求1的方法，其中分离工艺将使得吸附剂具有至少80％的烧失量(LOI)。
12.权利要求1的方法，其中通过一次或多次重力分离、静电分离、摩擦电分离、泡沫浮选分离、磁性分离和粒子大小分类，将非炭粒子从飞尘中除去来形成炭吸附剂。
13.权利要求1的方法，其中通过重力分离和随后的静电分离，将非炭粒子从飞尘中除去来形成炭吸附剂。
14.权利要求1的方法，其中通过泡沫浮选法和随后的研磨及其随后的附加的泡沫浮选法，将非炭粒子从飞尘中除去，来形成炭吸附剂。
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US09/167,790 | 1998-10-07 | ||
| US09/167,790 US6027551A (en) | 1998-10-07 | 1998-10-07 | Control of mercury emissions using unburned carbon from combustion by-products |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1332652A true CN1332652A (zh) | 2002-01-23 |
| CN1135134C CN1135134C (zh) | 2004-01-21 |
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| Application Number | Title | Priority Date | Filing Date |
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| CNB998133639A Expired - Fee Related CN1135134C (zh) | 1998-10-07 | 1999-10-05 | 利用燃烧副产物未燃烧的炭控制汞的排放 |
Country Status (8)
| Country | Link |
|---|---|
| US (1) | US6027551A (zh) |
| EP (1) | EP1185354A4 (zh) |
| CN (1) | CN1135134C (zh) |
| AU (1) | AU774284B2 (zh) |
| BR (1) | BR9915022A (zh) |
| IL (1) | IL142527A (zh) |
| MX (1) | MXPA01003785A (zh) |
| WO (1) | WO2000020100A1 (zh) |
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| CN1943842B (zh) * | 2004-10-08 | 2012-05-16 | 阿尔斯托姆科技有限公司 | 对固体燃料燃烧中汞排放的控制 |
| CN102698598A (zh) * | 2012-05-21 | 2012-10-03 | 华中科技大学 | 利用飞灰中的磁珠催化氧化烟气中单质汞的方法及设备 |
| CN102980175A (zh) * | 2012-11-29 | 2013-03-20 | 广东电网公司电力科学研究院 | 降低煤燃烧中单质汞排放量的装置及方法 |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1798599B (zh) * | 2003-06-03 | 2010-05-05 | 阿尔斯托姆科技有限公司 | 固体燃料燃烧的烟道气的脱汞方法和装置 |
| CN1943842B (zh) * | 2004-10-08 | 2012-05-16 | 阿尔斯托姆科技有限公司 | 对固体燃料燃烧中汞排放的控制 |
| CN102698598A (zh) * | 2012-05-21 | 2012-10-03 | 华中科技大学 | 利用飞灰中的磁珠催化氧化烟气中单质汞的方法及设备 |
| CN102698598B (zh) * | 2012-05-21 | 2014-08-27 | 华中科技大学 | 利用飞灰中的磁珠催化氧化烟气中单质汞的方法及设备 |
| CN102980175A (zh) * | 2012-11-29 | 2013-03-20 | 广东电网公司电力科学研究院 | 降低煤燃烧中单质汞排放量的装置及方法 |
| CN102980175B (zh) * | 2012-11-29 | 2015-11-18 | 广东电网公司电力科学研究院 | 降低煤燃烧中单质汞排放量的装置及方法 |
Also Published As
| Publication number | Publication date |
|---|---|
| WO2000020100A1 (en) | 2000-04-13 |
| AU6507499A (en) | 2000-04-26 |
| EP1185354A1 (en) | 2002-03-13 |
| US6027551A (en) | 2000-02-22 |
| AU774284B2 (en) | 2004-06-24 |
| EP1185354A4 (en) | 2003-02-05 |
| CN1135134C (zh) | 2004-01-21 |
| IL142527A (en) | 2004-06-20 |
| IL142527A0 (en) | 2002-03-10 |
| BR9915022A (pt) | 2002-01-15 |
| MXPA01003785A (es) | 2004-08-12 |
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